首页 > 最新文献

Inorganic Chemistry Frontiers最新文献

英文 中文
Low-content Ru–Pt supported on oxygen vacancy enriched black TiO2 with strong electronic interactions as efficient hydrogen generation electrocatalysts 以具有强电子相互作用的富氧空位黑色 TiO2 为载体的低含量 Ru-Pt 作为高效制氢电催化剂
IF 7 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-16 DOI: 10.1039/d4qi00919c
Yuanzong Shen, Weichen Li, Wenna Wang, Liantao Xin, Weiping Xiao, Guangrui Xu, Dehong Chen, Lei Wang, Fusheng Liu, Zexing Wu
Vacancy-engineered titanium dioxide (TiO2) loaded with low content noble metals is an important approach to achieve satisfactory hydrogen evolution reaction (HER) performance, but synthetic avenues are generally energy-intensive and tedious. Herein, a simple and ultrafast (60 s) microwave quasi-solid strategy is developed to prepare oxygen vacancy-enriched TiO2 doped with phosphorus to support low-loading Ru and Pt (Ru–Pt/P–TiO2−x) for the HER. The generated oxygen vacancies and introduced phosphorus favor a decrease in electrical resistance and enhance the metal–support interactions. Then, the as-developed Ru–Pt/P–TiO2−x exhibits satisfactory catalytic performance with an overpotential of 14 mV at 10 mA cm−2 and a small Tafel slope of 28 mV dec−1. In addition, the mass activity of Ru–Pt/P–TiO2−x is ten times or even hundred times higher than those of Ru/C and Pt/C. This study offers a novel and general approach to synthesize Ti-based compounds in renewable energy-related fields.
负载低含量贵金属的空位工程二氧化钛(TiO2)是实现令人满意的氢进化反应(HER)性能的重要方法,但合成途径通常耗能且繁琐。本文开发了一种简单、超快(60 秒)的微波准固体策略,用于制备掺杂磷的富氧空位二氧化钛,以支持氢进化反应中的低负载 Ru 和 Pt(Ru-Pt/P-TiO2-x)。生成的氧空位和引入的磷有利于降低电阻并增强金属与支撑物之间的相互作用。开发的 Ru-Pt/P-TiO2-x 在 10 mA cm-2 时的过电位为 14 mV,Tafel 斜率为 28 mV dec-1,表现出令人满意的催化性能。此外,Ru-Pt/P-TiO2-x 的质量活性是 Ru/C 和 Pt/C 的十倍甚至百倍。这项研究为在可再生能源相关领域合成钛基化合物提供了一种新颖而通用的方法。
{"title":"Low-content Ru–Pt supported on oxygen vacancy enriched black TiO2 with strong electronic interactions as efficient hydrogen generation electrocatalysts","authors":"Yuanzong Shen, Weichen Li, Wenna Wang, Liantao Xin, Weiping Xiao, Guangrui Xu, Dehong Chen, Lei Wang, Fusheng Liu, Zexing Wu","doi":"10.1039/d4qi00919c","DOIUrl":"https://doi.org/10.1039/d4qi00919c","url":null,"abstract":"Vacancy-engineered titanium dioxide (TiO<small><sub>2</sub></small>) loaded with low content noble metals is an important approach to achieve satisfactory hydrogen evolution reaction (HER) performance, but synthetic avenues are generally energy-intensive and tedious. Herein, a simple and ultrafast (60 s) microwave quasi-solid strategy is developed to prepare oxygen vacancy-enriched TiO<small><sub>2</sub></small> doped with phosphorus to support low-loading Ru and Pt (Ru–Pt/P–TiO<small><sub>2−<em>x</em></sub></small>) for the HER. The generated oxygen vacancies and introduced phosphorus favor a decrease in electrical resistance and enhance the metal–support interactions. Then, the as-developed Ru–Pt/P–TiO<small><sub>2−<em>x</em></sub></small> exhibits satisfactory catalytic performance with an overpotential of 14 mV at 10 mA cm<small><sup>−2</sup></small> and a small Tafel slope of 28 mV dec<small><sup>−1</sup></small>. In addition, the mass activity of Ru–Pt/P–TiO<small><sub>2−<em>x</em></sub></small> is ten times or even hundred times higher than those of Ru/C and Pt/C. This study offers a novel and general approach to synthesize Ti-based compounds in renewable energy-related fields.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141624740","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Halide-Driven Polarity Tuning and Optimized SHG-Bandgap Balance in (C4H11N2)ZnX3 (X = Cl, Br, I) (C4H11N2)ZnX3(X = Cl、Br、I)中卤化物驱动的极性调谐和优化的 SHG-带隙平衡
IF 7 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-16 DOI: 10.1039/d4qi01515k
Jin Chen, Huai-Yu Wu, Miao-Bin Xu, Ming-Chang Wang, Qian-Qian Chen, Bing-Xuan Li, Chun-Li Hu, Kezhao Du
In the quest for organic-inorganic metal halides (OIMHs) that harmoniously combine large second harmonic generation (SHG) efficiency with broad bandgaps, our study introduces a series of noncentrosymmetric and polar piperazine zinc halides, (C4H11N2)ZnX3 (X = Cl, Br, I). The distinct influence of halide anion size on the configuration of ZnNX3 tetrahedra is uncovered, revealing a design principle for enhancing SHG activity and manipulating bandgap characteristics. Specifically, (C4H11N2)ZnCl3 is the first example of deep-ultraviolet (deep-UV) nonlinear optical (NLO) OIMHs, with UV transparency lower that 190 nm and moderate SHG effect (0.8 times KDP). Meanwhile, comparaed with (C4H11N2)ZnI3 (2.1 times KDP, 4.52 eV), (C4H11N2)ZnBr3 boasts a widened bandgap of 5.53 eV while maintaining a striking SHG response (2.5 times KDP), representing a pinnacle in the SHG-bandgap balance among OIMHs with Eg exceeding 5.0 eV. Computational analyses underscore the critical roles of halide orbitals and ZnNX3 distortions in dictating SHG efficiency, with increasing halide polarizability correlating with heightened SHG contributions. This study paves the way for a novel approach to designing short-UV NLO crystals based on OIMHs.
为了寻找能将高二次谐波发生(SHG)效率与宽带隙和谐地结合在一起的有机无机金属卤化物(OIMHs),我们的研究引入了一系列非五次对称的极性哌嗪卤化锌--(C4H11N2)ZnX3(X = Cl、Br、I)。研究揭示了卤化物阴离子的大小对 ZnNX3 四面体构型的独特影响,揭示了增强 SHG 活性和操纵带隙特性的设计原理。具体来说,(C4H11N2)ZnCl3 是首个深紫外非线性光学(NLO)OIMHs 的实例,其紫外透明度低于 190 纳米,具有适度的 SHG 效应(0.8 倍 KDP)。同时,与(C4H11N2)ZnI3(2.1 倍 KDP,4.52 eV)相比,(C4H11N2)ZnBr3 的带隙扩大到 5.53 eV,同时保持了惊人的 SHG 响应(2.5 倍 KDP),代表了 Eg 超过 5.0 eV 的 OIMH 在 SHG 带隙平衡方面的巅峰。计算分析强调了卤化物轨道和 ZnNX3 扭曲在决定 SHG 效率方面的关键作用,卤化物极化率的增加与 SHG 贡献的增加相关。这项研究为基于 OIMHs 设计短紫外 NLO 晶体的新方法铺平了道路。
{"title":"Halide-Driven Polarity Tuning and Optimized SHG-Bandgap Balance in (C4H11N2)ZnX3 (X = Cl, Br, I)","authors":"Jin Chen, Huai-Yu Wu, Miao-Bin Xu, Ming-Chang Wang, Qian-Qian Chen, Bing-Xuan Li, Chun-Li Hu, Kezhao Du","doi":"10.1039/d4qi01515k","DOIUrl":"https://doi.org/10.1039/d4qi01515k","url":null,"abstract":"In the quest for organic-inorganic metal halides (OIMHs) that harmoniously combine large second harmonic generation (SHG) efficiency with broad bandgaps, our study introduces a series of noncentrosymmetric and polar piperazine zinc halides, (C4H11N2)ZnX3 (X = Cl, Br, I). The distinct influence of halide anion size on the configuration of ZnNX3 tetrahedra is uncovered, revealing a design principle for enhancing SHG activity and manipulating bandgap characteristics. Specifically, (C4H11N2)ZnCl3 is the first example of deep-ultraviolet (deep-UV) nonlinear optical (NLO) OIMHs, with UV transparency lower that 190 nm and moderate SHG effect (0.8 times KDP). Meanwhile, comparaed with (C4H11N2)ZnI3 (2.1 times KDP, 4.52 eV), (C4H11N2)ZnBr3 boasts a widened bandgap of 5.53 eV while maintaining a striking SHG response (2.5 times KDP), representing a pinnacle in the SHG-bandgap balance among OIMHs with Eg exceeding 5.0 eV. Computational analyses underscore the critical roles of halide orbitals and ZnNX3 distortions in dictating SHG efficiency, with increasing halide polarizability correlating with heightened SHG contributions. This study paves the way for a novel approach to designing short-UV NLO crystals based on OIMHs.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141624741","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Utilizing the magnetic properties of electrodes and magnetic fields in electrocatalysis 在电催化过程中利用电极和磁场的磁性能
IF 7 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-16 DOI: 10.1039/d4qi01296h
Nawaraj Karki, Fredrick Mufoyongo, Andrew J Wilson
Progress in understanding and controlling electrocatalytic reactions will enable electrochemistry to have a prominent role in our future energy economy in diverse sectors such as batteries, fuel cells, and electrolyzers. Complementary to advancements made by materials chemistry, surface chemistry, and engineering in electrocatalytic systems, magnetic fields have recently been reexplored as a handle to improve the activity and selectivity metrics in electrocatalytic reactions. The intrinsic magnetism of electrocatalysts and external magnetic fields can be utilized to introduce new reaction pathways and enhance electrocatalytic activity. In this review, we first provide a brief introduction to the primary mechanisms by which magnetic fields have been postulated to affect and enhance electrochemical reactions. We then discuss select literature examples that demonstrate improvements in electrocatalytic energy conversion and storage reactions in the presence of magnetic fields. Literature reports and magnetic field effects are organized by the magnetic properties of electrocatalysts: diamagnetic, paramagnetic, ferromagnetic, and antiferromagnetic. With the growing number of reports on magneto-electrocatalysis, we anticipate that magnetic fields will enable new discoveries and greater tunability in electrocatalysis including and beyond energy-relevant chemistry.
在理解和控制电催化反应方面取得的进展将使电化学在未来能源经济的电池、燃料电池和电解槽等不同领域中发挥重要作用。除了材料化学、表面化学和工程学在电催化系统方面取得的进展之外,磁场最近也被重新探讨,作为提高电催化反应活性和选择性指标的一种手段。电催化剂的内在磁性和外部磁场可用于引入新的反应途径并提高电催化活性。在本综述中,我们首先简要介绍了磁场影响和增强电化学反应的主要机制。然后,我们将讨论一些文献实例,这些实例证明了在磁场存在的情况下,电催化能量转换和储存反应的改善。文献报告和磁场效应按照电催化剂的磁性:二磁性、顺磁性、铁磁性和反铁磁性进行分类。随着有关磁电催化的报道越来越多,我们预计磁场将为电催化领域带来新的发现和更大的可调性,包括和超越能源相关的化学。
{"title":"Utilizing the magnetic properties of electrodes and magnetic fields in electrocatalysis","authors":"Nawaraj Karki, Fredrick Mufoyongo, Andrew J Wilson","doi":"10.1039/d4qi01296h","DOIUrl":"https://doi.org/10.1039/d4qi01296h","url":null,"abstract":"Progress in understanding and controlling electrocatalytic reactions will enable electrochemistry to have a prominent role in our future energy economy in diverse sectors such as batteries, fuel cells, and electrolyzers. Complementary to advancements made by materials chemistry, surface chemistry, and engineering in electrocatalytic systems, magnetic fields have recently been reexplored as a handle to improve the activity and selectivity metrics in electrocatalytic reactions. The intrinsic magnetism of electrocatalysts and external magnetic fields can be utilized to introduce new reaction pathways and enhance electrocatalytic activity. In this review, we first provide a brief introduction to the primary mechanisms by which magnetic fields have been postulated to affect and enhance electrochemical reactions. We then discuss select literature examples that demonstrate improvements in electrocatalytic energy conversion and storage reactions in the presence of magnetic fields. Literature reports and magnetic field effects are organized by the magnetic properties of electrocatalysts: diamagnetic, paramagnetic, ferromagnetic, and antiferromagnetic. With the growing number of reports on magneto-electrocatalysis, we anticipate that magnetic fields will enable new discoveries and greater tunability in electrocatalysis including and beyond energy-relevant chemistry.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141624744","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cation and anion co-partial substitution induced centrosymmetric to noncentrosymmetric structural transformation to construct nonlinear-optical rare-earth oxythiogermanates 阳离子和阴离子共同部分置换诱导中心对称到非中心对称的结构转变,从而构建非线性光学稀土氧硫锗酸盐
IF 7 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-16 DOI: 10.1039/d4qi01195c
Nan Zhang, Mei Yang, Wen-Dong Yao, Wei Xu, Wenfeng Zhou, Wenlong Liu, Sheng-Ping Guo
Rational structural design and modification based on known compounds is an effective strategy to explore new nonlinear optical (NLO) materials. Here, three new rare-earth (RE) oxythiogermanates Eu18Ge9O5S31 (1), Ca3.32Eu14.68Ge9O5S31 (2) and Ba3Eu15Ge9O5S31 (3) were obtained by the novel cation and anion co-partial substitution strategy from the parent β-Eu2GeS4 (0), which induces centrosymmetric to noncentrosymmetric (NCS) structural transformation and NLO activities. They crystallize with a pseudo-zero dimensional structure in the chiral R3 space group, featuring almost linearly arranged isolated GeS4 and GeOS3 tetrahedra. Their optical band gaps were determined to be 2.18, 2.23 and 2.24 eV, respectively. 1 and 2 show balanced NLO properties with moderate second-harmonic generation (SHG) responses (0.5 and 0.6 × AGS) and high laser-induced damage thresholds (LIDTs) (3.3 × AGS). Moreover, theoretical calculations show that their NLO properties are determined by the synergistic effect of GeS4 and GeOS3 tetrahedra. This work enriches the chemistry of rarely studied RE oxychalcogenides and provides a fresh route for designing NCS structures targeting diverse applications.
基于已知化合物的合理结构设计和改性是探索新型非线性光学(NLO)材料的有效策略。本文通过新型阳离子和阴离子共部分取代策略,从母体 β-Eu2GeS4 (0) 中获得了三种新的稀土(RE)氧硫锗酸盐 Eu18Ge9O5S31 (1)、Ca3.32Eu14.68Ge9O5S31 (2) 和 Ba3Eu15Ge9O5S31 (3),从而诱导了中心对称到非中心对称(NCS)的结构转变和 NLO 活性。它们在手性 R3 空间群中结晶出假零维结构,具有几乎线性排列的孤立 GeS4 和 GeOS3 四面体。经测定,它们的光带隙分别为 2.18、2.23 和 2.24 eV。1 和 2 显示出均衡的 NLO 特性,具有适度的二次谐波发生(SHG)响应(0.5 和 0.6 × AGS)和较高的激光诱导损伤阈值(LIDTs)(3.3 × AGS)。此外,理论计算表明,它们的 NLO 特性是由 GeS4 和 GeOS3 四面体的协同效应决定的。这项研究丰富了很少被研究的 RE 氧钙化物的化学性质,为设计针对不同应用的 NCS 结构提供了一条新的途径。
{"title":"Cation and anion co-partial substitution induced centrosymmetric to noncentrosymmetric structural transformation to construct nonlinear-optical rare-earth oxythiogermanates","authors":"Nan Zhang, Mei Yang, Wen-Dong Yao, Wei Xu, Wenfeng Zhou, Wenlong Liu, Sheng-Ping Guo","doi":"10.1039/d4qi01195c","DOIUrl":"https://doi.org/10.1039/d4qi01195c","url":null,"abstract":"Rational structural design and modification based on known compounds is an effective strategy to explore new nonlinear optical (NLO) materials. Here, three new rare-earth (RE) oxythiogermanates Eu<small><sub>18</sub></small>Ge<small><sub>9</sub></small>O<small><sub>5</sub></small>S<small><sub>31</sub></small> (<strong>1</strong>), Ca<small><sub>3.32</sub></small>Eu<small><sub>14.68</sub></small>Ge<small><sub>9</sub></small>O<small><sub>5</sub></small>S<small><sub>31</sub></small> (<strong>2</strong>) and Ba<small><sub>3</sub></small>Eu<small><sub>15</sub></small>Ge<small><sub>9</sub></small>O<small><sub>5</sub></small>S<small><sub>31</sub></small> (<strong>3</strong>) were obtained by the novel cation and anion co-partial substitution strategy from the parent β-Eu<small><sub>2</sub></small>GeS<small><sub>4</sub></small> (<strong>0</strong>), which induces centrosymmetric to noncentrosymmetric (NCS) structural transformation and NLO activities. They crystallize with a <em>pseudo</em>-zero dimensional structure in the chiral <em>R</em>3 space group, featuring almost linearly arranged isolated GeS<small><sub>4</sub></small> and GeOS<small><sub>3</sub></small> tetrahedra. Their optical band gaps were determined to be 2.18, 2.23 and 2.24 eV, respectively. <strong>1</strong> and <strong>2</strong> show balanced NLO properties with moderate second-harmonic generation (SHG) responses (0.5 and 0.6 × AGS) and high laser-induced damage thresholds (LIDTs) (3.3 × AGS). Moreover, theoretical calculations show that their NLO properties are determined by the synergistic effect of GeS<small><sub>4</sub></small> and GeOS<small><sub>3</sub></small> tetrahedra. This work enriches the chemistry of rarely studied RE oxychalcogenides and provides a fresh route for designing NCS structures targeting diverse applications.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141624742","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Easy Recycling of Nanoscale Fe2O3-Based Catalysts for Nitroarene Reduction to Anilines by Pyrolysis of Metallogel 通过热解金属凝胶轻松回收利用基于纳米级 Fe2O3 的催化剂将硝基炔还原为苯胺
IF 7 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-16 DOI: 10.1039/d4qi01250j
Wen-Ting Deng, Xiang Zhong, Yang Li, Xin-Jian Jia, Haiqing Luo, Xuzhong Luo
A organic gelator N4, N4'-di(pyridin-3-yl)-[2, 2'-bipyridine]-4, 4'-dicarboxamide and Fe3+ are used to self-assemble to form a new metallogel Fe-2B-N3 by under mild conditions, whose structure and properties can be proved by NMR, MS and rheology. And further pyrolysis the metallogel Fe-2B-N3 to obtain a high-performance Fe2O3-based heterogeneous catalytic material L that characterized by X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Transmission Electron Microscope (TEM) and Specific Surface Area Analyzer (BET). The catalytic material L shows good catalytic performance and stability for the reduction of nitroaromatic compounds (NACs) to amine compounds. Especially under mild and simple conditions, p-chloronitrobenzene can be reduced to p-chloroaniline in 10 minutes, with a conversion rate of over 99%. Furthermore, the catalytic material L was simply, highly recycle and thus expands the application of metallogel.
利用有机凝胶剂 N4、N4'-二(吡啶-3-基)-[2,2'-联吡啶]-4,4'-二甲酰胺和 Fe3+ 在温和条件下自组装形成新的金属凝胶 Fe-2B-N3,其结构和性质可通过核磁共振、质谱和流变学得到证明。通过 X 射线粉末衍射 (XRD)、X 射线光电子能谱 (XPS)、透射电子显微镜 (TEM) 和比表面积分析仪 (BET) 对其进行表征。催化材料 L 在将硝基芳香族化合物还原成胺类化合物的过程中表现出良好的催化性能和稳定性。特别是在温和简单的条件下,对氯硝基苯可在 10 分钟内还原成对氯苯胺,转化率超过 99%。此外,催化材料 L 易于回收利用,因此扩大了金属凝胶的应用范围。
{"title":"Easy Recycling of Nanoscale Fe2O3-Based Catalysts for Nitroarene Reduction to Anilines by Pyrolysis of Metallogel","authors":"Wen-Ting Deng, Xiang Zhong, Yang Li, Xin-Jian Jia, Haiqing Luo, Xuzhong Luo","doi":"10.1039/d4qi01250j","DOIUrl":"https://doi.org/10.1039/d4qi01250j","url":null,"abstract":"A organic gelator N<small><sup>4</sup></small>, N<small><sup>4'</sup></small>-di(pyridin-3-yl)-[2, 2'-bipyridine]-4, 4'-dicarboxamide and Fe<small><sup>3+</sup></small> are used to self-assemble to form a new metallogel Fe-2B-N3 by under mild conditions, whose structure and properties can be proved by NMR, MS and rheology. And further pyrolysis the metallogel Fe-2B-N3 to obtain a high-performance Fe<small><sub>2</sub></small>O<small><sub>3</sub></small>-based heterogeneous catalytic material L that characterized by X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Transmission Electron Microscope (TEM) and Specific Surface Area Analyzer (BET). The catalytic material L shows good catalytic performance and stability for the reduction of nitroaromatic compounds (NACs) to amine compounds. Especially under mild and simple conditions, p-chloronitrobenzene can be reduced to p-chloroaniline in 10 minutes, with a conversion rate of over 99%. Furthermore, the catalytic material L was simply, highly recycle and thus expands the application of metallogel.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141624743","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Tunable SIM properties in a family of 3D anilato-based Lanthanide-MOFs 基于苯胺的三维镧系元素-MOF 家族的可调 SIM 特性
IF 7 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-16 DOI: 10.1039/d4qi01549e
Noemi N. Monni, Sourav Dey, Víctor García-López, Mariangela M. Oggianu, José J. Baldoví, Maria Laura Mercuri, Miguel Clemente Leon, Eugenio Coronado
By reacting 3,6-ditriazolyl-2,5-dihydroxybenzoquinone (H2trz2An) anilato linker with LnIII ions (LnIII = Dy, Tb, Ho), two different series of polymorphs, formulated as [Ln2(trz2An)3(H2O)4]n·10H2O (DyIII, 1a; TbIII, 2a, HoIII, 3a) and [Ln2(trz2An)3(H2O)4]n·7H2O (DyIII, 1b, TbIII, 2b, HoIII, 3b) have been obtained. In these series the two DyIII-coordination networks (1a and 1b) and the TbIII-coordination polymer (2b) show a Single Ion Magnet (SIM) behavior. 1-3a MOFs show reversible structural flexibility upon removal of a coordinated water molecule from a distorted hexagonal 2D framework to a distorted 3,6-brickwall rectangular 3D structure in [Ln2(trz2An)3(H2O)2]n·2H2O (DyIII, 1a_des; TbIII, 2a_des, HoIII, 3a_des) involving shrinkage/expansion of the hexagonal-rectangular networks. Noteworthy, 2b represents the first example of TbIII–anilate-based coordination polymer showing SIM behaviour to date and the best SIM properties within the polymorphs. Theoretical investigation via ab initio CASSCF calculations supports this behavior, since 2b shows less mixing between the mJ states of the ground state among all the studied complexes.
通过将 3,6-二氮唑基-2,5-二羟基苯醌(H2trz2An)苯胺基连接体与 LnIII 离子(LnIII = Dy、Tb、Ho)反应,产生了两种不同系列的多晶体,分别为 [Ln2(trz2An)3(H2O)4]n-10H2O (DyIII,1a;TbIII,2a;HoIII,3a)和 [Ln2(trz2An)3(H2O)4]n-7H2O (DyIII,1b;TbIII,2b;HoIII,3a);TbIII,2a;HoIII,3a)和 [Ln2(trz2An)3(H2O)4]n-7H2O(DyIII,1b;TbIII,2b;HoIII,3b)。在这些系列中,两个 DyIII 配位网络(1a 和 1b)和 TbIII 配位聚合物(2b)显示出单离子磁体(SIM)行为。在[Ln2(trz2An)3(H2O)2]n-2H2O(DyIII,1a_des;TbIII,2a_des;HoIII,3a_des)中,当去除配位水分子后,[Ln2(trz2An)3(H2O)2]n-2H2O(DyIII,1a_des;TbIII,2a_des;HoIII,3a_des)从扭曲的六角形二维框架变为扭曲的 3,6 砖墙矩形三维结构,显示出可逆的结构灵活性,其中涉及六角形-矩形网络的收缩/扩张。值得注意的是,2b 是迄今为止第一个显示 SIM 行为的 TbIII-苯胺基配位聚合物实例,也是多晶型中 SIM 性能最好的聚合物。通过 ab initio CASSCF 计算进行的理论研究也支持这种行为,因为在所有研究的复合物中,2b 的基态 mJ 状态之间的混合较少。
{"title":"Tunable SIM properties in a family of 3D anilato-based Lanthanide-MOFs","authors":"Noemi N. Monni, Sourav Dey, Víctor García-López, Mariangela M. Oggianu, José J. Baldoví, Maria Laura Mercuri, Miguel Clemente Leon, Eugenio Coronado","doi":"10.1039/d4qi01549e","DOIUrl":"https://doi.org/10.1039/d4qi01549e","url":null,"abstract":"By reacting 3,6-ditriazolyl-2,5-dihydroxybenzoquinone (H2trz2An) anilato linker with LnIII ions (LnIII = Dy, Tb, Ho), two different series of polymorphs, formulated as [Ln2(trz2An)3(H2O)4]n·10H2O (DyIII, 1a; TbIII, 2a, HoIII, 3a) and [Ln2(trz2An)3(H2O)4]n·7H2O (DyIII, 1b, TbIII, 2b, HoIII, 3b) have been obtained. In these series the two DyIII-coordination networks (1a and 1b) and the TbIII-coordination polymer (2b) show a Single Ion Magnet (SIM) behavior. 1-3a MOFs show reversible structural flexibility upon removal of a coordinated water molecule from a distorted hexagonal 2D framework to a distorted 3,6-brickwall rectangular 3D structure in [Ln2(trz2An)3(H2O)2]n·2H2O (DyIII, 1a_des; TbIII, 2a_des, HoIII, 3a_des) involving shrinkage/expansion of the hexagonal-rectangular networks. Noteworthy, 2b represents the first example of TbIII–anilate-based coordination polymer showing SIM behaviour to date and the best SIM properties within the polymorphs. Theoretical investigation via ab initio CASSCF calculations supports this behavior, since 2b shows less mixing between the mJ states of the ground state among all the studied complexes.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141624745","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Integrating surface modification to improve the electrochemical performance of Li-rich cathode materials 结合表面改性提高富锂阴极材料的电化学性能
IF 7 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-16 DOI: 10.1039/d4qi00769g
Xiaoyuan Zhang, Yanxiao Gao, Xiangnan Li, Wenfeng Liu, Huishuang Zhang, Shuting Yang, Yanhong Yin
Li-rich cathode materials (LLO) exhibit a high specific capacity, but their application is impeded by their poor cycling stability and rate performance which arises from the irreversible anionic redox reaction and their poor electrical conductivity. In this regard, a simple phytic acid surface treatment technique was employed to form an integrated surface structure comprising Li3PO4 and oxygen vacancies (Vos) on the surface of LLO materials. In particular, the effect of the Li3PO4 layer on the defect structure and their synergistic effect on the electrochemical performances of LLO were researched through experimental and theoretical calculations. The results prove that the existence of Li3PO4 can improve the Vo content obviously. The coating layer and the synchronously formed Vo can also facilitate Li+ diffusion, improve the electrical conductivity, and inhibit the irreversible O2 release effectively, thus increasing the cycling stability and rate performance of LLO. Consequently, the initial coulombic efficiency (ICE) increases from 62.8% to 72%. After 200 cycles at 0.5C, the capacity retention has improved significantly from 78% to 92.3%, accompanied by a minimal voltage fading value of 108.8 mV. The discharge specific capacity still reaches 125 mA h g−1 even at a current density of 5C. This work proves the effect of the Li3PO4 coating layer on the defect structure and electrochemical properties of the LLO material and provides an effective clue to improve its performance.
富锂阴极材料(LLO)具有很高的比容量,但由于其不可逆的阴离子氧化还原反应和较差的导电性,导致其循环稳定性和速率性能较差,从而阻碍了其应用。为此,我们采用了一种简单的植酸表面处理技术,在 LLO 材料表面形成了由 Li3PO4 和氧空位(Vos)组成的一体化表面结构。其中,通过实验和理论计算研究了 Li3PO4 层对缺陷结构的影响及其对 LLO 电化学性能的协同作用。结果证明,Li3PO4 的存在能明显提高 Vo 含量。涂层和同步形成的 Vo 还能促进 Li+ 扩散,提高导电性,有效抑制不可逆 O2 释放,从而提高 LLO 的循环稳定性和速率性能。因此,初始库仑效率(ICE)从 62.8% 提高到 72%。在 0.5C 下循环 200 次后,容量保持率从 78% 显著提高到 92.3%,电压衰减值降至 108.8 mV。即使在 5C 的电流密度下,放电比容量仍能达到 125 mA h g-1。这项工作证明了 Li3PO4 涂层对 LLO 材料缺陷结构和电化学性能的影响,并为提高其性能提供了有效的线索。
{"title":"Integrating surface modification to improve the electrochemical performance of Li-rich cathode materials","authors":"Xiaoyuan Zhang, Yanxiao Gao, Xiangnan Li, Wenfeng Liu, Huishuang Zhang, Shuting Yang, Yanhong Yin","doi":"10.1039/d4qi00769g","DOIUrl":"https://doi.org/10.1039/d4qi00769g","url":null,"abstract":"Li-rich cathode materials (LLO) exhibit a high specific capacity, but their application is impeded by their poor cycling stability and rate performance which arises from the irreversible anionic redox reaction and their poor electrical conductivity. In this regard, a simple phytic acid surface treatment technique was employed to form an integrated surface structure comprising Li<small><sub>3</sub></small>PO<small><sub>4</sub></small> and oxygen vacancies (Vos) on the surface of LLO materials. In particular, the effect of the Li<small><sub>3</sub></small>PO<small><sub>4</sub></small> layer on the defect structure and their synergistic effect on the electrochemical performances of LLO were researched through experimental and theoretical calculations. The results prove that the existence of Li<small><sub>3</sub></small>PO<small><sub>4</sub></small> can improve the Vo content obviously. The coating layer and the synchronously formed Vo can also facilitate Li<small><sup>+</sup></small> diffusion, improve the electrical conductivity, and inhibit the irreversible O<small><sub>2</sub></small> release effectively, thus increasing the cycling stability and rate performance of LLO. Consequently, the initial coulombic efficiency (ICE) increases from 62.8% to 72%. After 200 cycles at 0.5C, the capacity retention has improved significantly from 78% to 92.3%, accompanied by a minimal voltage fading value of 108.8 mV. The discharge specific capacity still reaches 125 mA h g<small><sup>−1</sup></small> even at a current density of 5C. This work proves the effect of the Li<small><sub>3</sub></small>PO<small><sub>4</sub></small> coating layer on the defect structure and electrochemical properties of the LLO material and provides an effective clue to improve its performance.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141624739","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Hierarchical porous carbon stabilized atomically dispersed Au catalyst for acetylene hydrochlorination 用于乙炔加氢氯化的分层多孔碳稳定原子分散金催化剂
IF 7 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-16 DOI: 10.1039/d4qi00756e
Guojun Lan, Jinlong Zhou, Qingfeng Ye, Di Lin, Yiyang Qiu, Zaizhe Cheng, Xiucheng Sun, Ying Li
Carbon-supported gold catalysts serve as sustainable alternatives to the toxic mercuric chloride catalyst in the industrial hydrochlorination of acetylene. The porosity and surface defects of catalytic materials have a significant impact on the performance of heterogeneous catalysts. Herein, a sheet-like carbon stabilized atomically dispersed Au catalyst (Au-CSC-850) with hierarchical porous nanostructure and extensive surface voids defects has been synthesized by one-step pyrolysis method using cationic starch as a carbon precursor. The irregular dispersion of surface void defects within the Au-CSC-850 catalyst effectively interconnects the nanochannels and enhances the adsorption capacity for acetylene molecules. The activity of the Au-CSC-850 catalyst is significantly enhanced by the hierarchical porous structure derived from cationic starch, in comparison to the microporous Au-SC-850 catalyst obtained from pristine starch. The Au-CSC-850 catalyst demonstrated exceptional stability in durability tests, as evidenced by the absence of any significant activity loss over a 200-hour long-term reaction period. This work elucidates the profound influence of porous nanostructures and void defects on the catalytic activity of acetylene hydrochlorination catalysts, offering a convenient approach to fabricate highly efficient carbon supported metal catalysts.
在乙炔的工业氢氯化过程中,碳支撑金催化剂是有毒氯化汞催化剂的可持续替代品。催化材料的孔隙率和表面缺陷对异相催化剂的性能有重大影响。本文以阳离子淀粉为碳前驱体,通过一步热分解法合成了具有分层多孔纳米结构和大量表面空隙缺陷的片状碳稳定原子分散金催化剂(Au-CSC-850)。Au-CSC-850 催化剂表面空隙缺陷的不规则分散有效地将纳米通道相互连接在一起,增强了对乙炔分子的吸附能力。与原始淀粉制备的微孔 Au-SC-850 催化剂相比,阳离子淀粉制备的分层多孔结构显著提高了 Au-CSC-850 催化剂的活性。Au-CSC-850 催化剂在耐久性测试中表现出了极高的稳定性,在 200 小时的长期反应过程中没有出现任何明显的活性损失就是证明。这项工作阐明了多孔纳米结构和空隙缺陷对乙炔加氢氯化催化剂催化活性的深刻影响,为制备高效的碳支撑金属催化剂提供了一种便捷的方法。
{"title":"Hierarchical porous carbon stabilized atomically dispersed Au catalyst for acetylene hydrochlorination","authors":"Guojun Lan, Jinlong Zhou, Qingfeng Ye, Di Lin, Yiyang Qiu, Zaizhe Cheng, Xiucheng Sun, Ying Li","doi":"10.1039/d4qi00756e","DOIUrl":"https://doi.org/10.1039/d4qi00756e","url":null,"abstract":"Carbon-supported gold catalysts serve as sustainable alternatives to the toxic mercuric chloride catalyst in the industrial hydrochlorination of acetylene. The porosity and surface defects of catalytic materials have a significant impact on the performance of heterogeneous catalysts. Herein, a sheet-like carbon stabilized atomically dispersed Au catalyst (Au-CSC-850) with hierarchical porous nanostructure and extensive surface voids defects has been synthesized by one-step pyrolysis method using cationic starch as a carbon precursor. The irregular dispersion of surface void defects within the Au-CSC-850 catalyst effectively interconnects the nanochannels and enhances the adsorption capacity for acetylene molecules. The activity of the Au-CSC-850 catalyst is significantly enhanced by the hierarchical porous structure derived from cationic starch, in comparison to the microporous Au-SC-850 catalyst obtained from pristine starch. The Au-CSC-850 catalyst demonstrated exceptional stability in durability tests, as evidenced by the absence of any significant activity loss over a 200-hour long-term reaction period. This work elucidates the profound influence of porous nanostructures and void defects on the catalytic activity of acetylene hydrochlorination catalysts, offering a convenient approach to fabricate highly efficient carbon supported metal catalysts.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141624749","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Catalysis for the hydrogenation of nitroaromatics by highly dispersed palladium nanoparticles anchored on a resorcin[4]arene-based metal–organic dimer containing amino groups 锚定在含有氨基的间苯二酚[4]炔基金属有机二聚体上的高分散钯纳米粒子对硝基芳烃氢化的催化作用
IF 7 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-15 DOI: 10.1039/d4qi01342e
Fei-Fei Wang, Wei Jiang, Wen-Yuan Pei, Jian-Fang Ma
We herein reported a design strategy for the construction of resorcin[4]arene-based metal–organic complexes through adjusting auxiliary linkers. By precisely tuning 1,4-benzenedicarboxylic acid analogs, a series of isostructural resorcin[4]arene-based metal–organic dimers, namely, [Zn4(TIC4R)2·(L)2·(OH)2]·2HCOO·solvent (1–9) (L = 1,4-benzenedicarboxylic acid analogs and TIC4R = tetra(imidazole)resorcin[4]arene), were rationally prepared under solvothermal conditions. Considering the amino groups on the backbone of dimer 2, Pd nanoparticles were prepared to uniformly disperse on the substrate of 2 to give Pd@2. Most importantly, the Pd@2 catalyst was applied for nitroarene hydrogenation with efficient catalytic performance and high selectivity under mild conditions. This work afforded a possible method for precisely controlling the target complex assemblies and their further application.
我们在此报告了一种通过调整辅助连接体来构建间苯二酚[4]炔基金属有机配合物的设计策略。通过精确调节 1,4-苯二甲酸类似物,在溶热条件下合理制备了一系列等结构的间苯二酚[4]炔基金属有机二聚体,即[Zn4(TIC4R)2-(L)2-(OH)2]-2HCOO-溶剂(1-9)(L = 1,4-苯二甲酸类似物,TIC4R = 四(咪唑)间苯二酚[4]炔)。考虑到二聚体 2 骨架上的氨基,制备了钯纳米粒子,使其均匀分散在二聚体 2 的基底上,得到 Pd@2。 最重要的是,Pd@2 催化剂被应用于硝基炔氢化反应,在温和条件下具有高效的催化性能和高选择性。这项工作为精确控制目标复合物组装及其进一步应用提供了一种可行的方法。
{"title":"Catalysis for the hydrogenation of nitroaromatics by highly dispersed palladium nanoparticles anchored on a resorcin[4]arene-based metal–organic dimer containing amino groups","authors":"Fei-Fei Wang, Wei Jiang, Wen-Yuan Pei, Jian-Fang Ma","doi":"10.1039/d4qi01342e","DOIUrl":"https://doi.org/10.1039/d4qi01342e","url":null,"abstract":"We herein reported a design strategy for the construction of resorcin[4]arene-based metal–organic complexes through adjusting auxiliary linkers. By precisely tuning 1,4-benzenedicarboxylic acid analogs, a series of isostructural resorcin[4]arene-based metal–organic dimers, namely, [Zn<small><sub>4</sub></small>(TIC4R)<small><sub>2</sub></small>·(L)<small><sub>2</sub></small>·(OH)<small><sub>2</sub></small>]·2HCOO·solvent (<strong>1–9</strong>) (L = 1,4-benzenedicarboxylic acid analogs and TIC4R = tetra(imidazole)resorcin[4]arene), were rationally prepared under solvothermal conditions. Considering the amino groups on the backbone of dimer <strong>2</strong>, Pd nanoparticles were prepared to uniformly disperse on the substrate of <strong>2</strong> to give <strong>Pd@2</strong>. Most importantly, the <strong>Pd@2</strong> catalyst was applied for nitroarene hydrogenation with efficient catalytic performance and high selectivity under mild conditions. This work afforded a possible method for precisely controlling the target complex assemblies and their further application.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141618229","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Rapid preparation of Fe coordination structure adjustable ORR catalyst by microwave with a half-wave potential above 0.9 V 用半波电位高于 0.9 V 的微波快速制备铁配位结构可调 ORR 催化剂
IF 7 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-07-15 DOI: 10.1039/d4qi00952e
Qingtao Wang, Xia Hu, Kai Cui, Yanxia Wu, Guofu Ma, Ziqiang Lei, Shufang Ren
Oxygen reduction reaction (ORR) catalyst is a crucial component of metal-air battery. Herein, modified carbon nanotubes are used to support iron phthalocyanine, followed by the fabrication of single-atom and cluster coexisting catalysts by fast microwave method. The two catalysts have Fe-N5 and Fe-P-N4 coordination structures, respectively. Electrochemical tests show that the FeNC/Fe-N5-C and FeNC/Fe-P-N4-C catalysts have half-wave potential of 0.906 and 0.886 V in alkaline solvent. The Zn-air battery prepared with the FeNC/Fe-N5-C catalyst has a specific capacity of 791 mA h g−1 and a maximum power density of 190 mW cm−2. DFT calculations show that the axial coordination bonds in FeNC/Fe-N5-C and FeNC/Fe-P-N4-C are conducive to accelerate the transfer of electron. The d-band centers of the axial coordination Fe-N5 and Fe-P-N4 are closer to the Fermi level, confirming that the presence of the axial coordination bonds enhances the adsorption of the reaction intermediates and reduces the ORR barriers.
氧还原反应(ORR)催化剂是金属-空气电池的重要组成部分。本文利用改性碳纳米管支撑酞菁铁,然后通过快速微波法制备了单原子和团簇共存催化剂。两种催化剂分别具有 Fe-N5 和 Fe-P-N4 配位结构。电化学测试表明,FeNC/Fe-N5-C 和 FeNC/Fe-P-N4-C 催化剂在碱性溶剂中的半波电位分别为 0.906 V 和 0.886 V。使用 FeNC/Fe-N5-C 催化剂制备的锌-空气电池的比容量为 791 mA h g-1,最大功率密度为 190 mW cm-2。DFT 计算表明,FeNC/Fe-N5-C 和 FeNC/Fe-P-N4-C 中的轴向配位键有利于加速电子转移。轴向配位 Fe-N5 和 Fe-P-N4 的 d 带中心更接近费米级,这证实了轴向配位键的存在增强了反应中间产物的吸附并降低了 ORR 的壁垒。
{"title":"Rapid preparation of Fe coordination structure adjustable ORR catalyst by microwave with a half-wave potential above 0.9 V","authors":"Qingtao Wang, Xia Hu, Kai Cui, Yanxia Wu, Guofu Ma, Ziqiang Lei, Shufang Ren","doi":"10.1039/d4qi00952e","DOIUrl":"https://doi.org/10.1039/d4qi00952e","url":null,"abstract":"Oxygen reduction reaction (ORR) catalyst is a crucial component of metal-air battery. Herein, modified carbon nanotubes are used to support iron phthalocyanine, followed by the fabrication of single-atom and cluster coexisting catalysts by fast microwave method. The two catalysts have Fe-N5 and Fe-P-N4 coordination structures, respectively. Electrochemical tests show that the FeNC/Fe-N5-C and FeNC/Fe-P-N4-C catalysts have half-wave potential of 0.906 and 0.886 V in alkaline solvent. The Zn-air battery prepared with the FeNC/Fe-N5-C catalyst has a specific capacity of 791 mA h g−1 and a maximum power density of 190 mW cm−2. DFT calculations show that the axial coordination bonds in FeNC/Fe-N5-C and FeNC/Fe-P-N4-C are conducive to accelerate the transfer of electron. The d-band centers of the axial coordination Fe-N5 and Fe-P-N4 are closer to the Fermi level, confirming that the presence of the axial coordination bonds enhances the adsorption of the reaction intermediates and reduces the ORR barriers.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141618226","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
期刊
Inorganic Chemistry Frontiers
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1