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Corrigendum to “Machine learning accelerated interfacial fluxionality in Ni-supported metal nitride ammonia synthesis catalysts” [J. Catal. 450 (2025) 116224] “机器学习加速ni负载金属氮氨合成催化剂的界面流动性”的勘误[J]。Catal. 450 (2025) 116224]
IF 7.3 1区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-10-24 DOI: 10.1016/j.jcat.2026.117238
Pranav Roy, Brandon C. Bukowski
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引用次数: 0
Visible-light-driven piezo-photocatalytic water purification by an SPR-enhanced Bi0.5Na0.5TiO3/Bi-QDs/BiOBr heterojunction: dye mineralization, detoxification, and bacterial disinfection spr增强Bi0.5Na0.5TiO3/Bi-QDs/BiOBr异质结的可见光压电催化水净化:染料矿化、解毒和细菌消毒
IF 7.3 1区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-10-24 DOI: 10.1016/j.jcat.2026.117243
Jing-yi Xie, Ming Yang, Hui Yu, Xiang-ting Dong, Ying Yang
Perovskite materials are a research hotspot in photocatalytic applications at present, yet their performances are constrained by the weak built-in electric field, high transfer resistance of interface charges, rapid recombination of charge carriers, wide bandgap (>3.0 eV), low utilization rate for visible light, few active sites, poor adsorption capacity for reactants and slow reaction kinetics. In view of these, this study employed in-situ reduction and interface engineering strategies to reduce Bi quantum dots (Bi-QDs) onto BiOBr nanoflowers and integrate with perovskite structure Bi0.5Na0.5TiO3 for forming Z-scheme heterojunctions. The piezoelectric effect, primarily from Bi0.5Na0.5TiO3 with a minor contribution from Bi-QDs/BiOBr, effectively enhances the built-in electric field and accelerates the migration of surface charges. The Z-scheme heterojunctions could enhance the separation efficiency of photogenerated charges and accelerate the reaction kinetics. Meanwhile, the surface plasmon resonance (SPR) effect of Bi-QDs enhances visible-light absorption and works synergistically with the piezoelectric field to promote charge separation. Remarkably, it achieved efficient degradation of RhB under outdoor sunlight conditions. This design achieves the synergy of the piezoelectric effect, photocatalytic action and SPR effect, which mitigates environmental defects in conventional lead-based perovskites, enhances interfacial interactions, improves separation efficiency of photogenerated charge carrier, and significantly enhances the catalytic performance of the material.
钙钛矿材料是目前光催化应用的研究热点,但其性能受到内置电场弱、界面电荷转移阻力大、载流子重组速度快、带隙宽(>3.0 eV)、可见光利用率低、活性位点少、对反应物吸附能力差、反应动力学慢等限制。鉴于此,本研究采用原位还原和界面工程策略将Bi量子点(Bi- qds)还原到BiOBr纳米花上,并与钙钛矿结构Bi0.5Na0.5TiO3集成形成Z-scheme异质结。压电效应主要来自Bi0.5Na0.5TiO3, Bi-QDs/BiOBr的贡献较小,有效增强了内置电场,加速了表面电荷的迁移。z型异质结可以提高光生电荷的分离效率,加快反应动力学。同时,双量子点的表面等离子体共振(SPR)效应增强了可见光吸收,并与压电场协同作用促进电荷分离。值得注意的是,它在室外光照条件下实现了RhB的高效降解。本设计实现了压电效应、光催化作用和SPR效应的协同作用,减轻了传统铅基钙钛矿的环境缺陷,增强了界面相互作用,提高了光生载流子的分离效率,显著提高了材料的催化性能。
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引用次数: 0
Ligand-engineered strategy stabilizing bismuth-based MOF heterointerfaces for selective electrocatalytic CO2 reduction to formate 配体工程策略稳定铋基MOF异质界面用于选择性电催化CO2还原生成甲酸
IF 7.3 1区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-10-23 DOI: 10.1016/j.jcat.2026.117240
Yiren Zhu, Wenli Bao, Peiran Wu, Jiansong Wang, Huizhuan Zhu, Chang Wang, Liu-Liu Shen, Gui-Rong Zhang, Donghai Mei
Bismuth-based catalysts are highly active for electrochemical CO2 reduction to formate, while their uncontrolled structural reconstruction under operating conditions, especially the deep reduction of the Bi/Bi2O2CO3 heterointerface to bulk Bi0 often leads to rapid loss of formate selectivity. Here we report a ligand-engineered coordination strategy that precisely dictates the dynamic structural evolution of bismuth-based metal–organic frameworks, enabling in situ formation of stabilized Bi/Bi2O2CO3 heterointerface. By introducing an asymmetric 1H-pyrazole-4-carboxylic acid ligand, a hierarchical coordination environment is constructed, featuring coexisting Bi-O and labile Bi-N bonds. Density functional theory calculations combined with operando spectroscopic measurements reveal that the weaker Bi-N linkages selectively dissociate under cathodic polarization, initiating a controlled and stepwise transformation into crystalline Bi2O2CO3 nanosheets. This ordered reconstruction yields uniformly dispersed metallic Bi domains (<10 nm) coupled with Bi2O2CO3, forming well-defined heterointerfaces that favor formate production. The catalyst achieves a formate Faradaic efficiency of 96.3 % at −0.99 V (vs. RHE) and maintains stable performance over 8 h. This work demonstrates that the pivotal role of asymmetric coordination design in precatalysts as a means to influence reconstruction pathways at the atomic scale, providing a versatile and innovative strategy for constructing robust, selective, and dynamically adaptive electrocatalysts.
铋基催化剂在电化学CO2还原生成甲酸方面具有高活性,但其在操作条件下不受控制的结构重构,特别是Bi/Bi2O2CO3异质界面深度还原生成大块Bi0,往往导致甲酸选择性的快速丧失。在这里,我们报告了一种配体工程配位策略,该策略精确地指示了铋基金属-有机框架的动态结构演变,使原位形成稳定的Bi/Bi2O2CO3异质界面。通过引入不对称的1h -吡唑-4-羧酸配体,构建了Bi-O和稳定Bi-N键共存的层次化配位环境。密度泛函理论计算与operando光谱测量相结合表明,较弱的Bi-N键在阴极极化下选择性地解离,开始可控的逐步转变为结晶Bi2O2CO3纳米片。这种有序的重建产生了均匀分散的金属Bi畴(<10 nm),与Bi2O2CO3偶联,形成了明确的异质界面,有利于生成甲酸盐。在−0.99 V(相对于RHE)下,催化剂的甲酸法拉第效率达到96.3% %,并在8 h内保持稳定的性能。这项工作证明了不对称配位设计在预催化剂中的关键作用,作为一种影响原子尺度上重建途径的手段,为构建鲁棒、选择性和动态自适应的电催化剂提供了一种通用和创新的策略。
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引用次数: 0
Heteroaryl-bridged binuclear nickel catalysts for chain-walking ethylene (co)polymerization 链走乙烯(co)聚合用杂芳基桥接双核镍催化剂
IF 7.3 1区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-10-23 DOI: 10.1016/j.jcat.2026.117245
Ruirui Zhang, Mengna Lei, Huanhuan Ma, Qian Miao, Xuhui Dai, Ziyang Tian, Naseer Ahmad, Chao Li, Muhammad Asadullah Khan, Fuzhou Wang
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引用次数: 0
Breaking the density-stability trade-off of isolated gallium sites for propane dehydrogenation 打破分离镓位在丙烷脱氢中的密度-稳定性权衡
IF 7.3 1区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-10-21 DOI: 10.1016/j.jcat.2026.117244
Fujing Nie, Yuan Kong, Si Chen, Xi Zhang, Guangyuan Xu, Yanzhe Ma, Dongyue Liu, Mengxin Wang, Lijin Gan, Yi Duan, Shibo Xi, Huan Yan
{"title":"Breaking the density-stability trade-off of isolated gallium sites for propane dehydrogenation","authors":"Fujing Nie, Yuan Kong, Si Chen, Xi Zhang, Guangyuan Xu, Yanzhe Ma, Dongyue Liu, Mengxin Wang, Lijin Gan, Yi Duan, Shibo Xi, Huan Yan","doi":"10.1016/j.jcat.2026.117244","DOIUrl":"https://doi.org/10.1016/j.jcat.2026.117244","url":null,"abstract":"","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"165 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149233027","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
Impact of polyvinyl chloride on the hydrogenolysis of low-density polyethylene over supported transition metal catalysts 聚氯乙烯对负载型过渡金属催化剂上低密度聚乙烯氢解反应的影响
IF 7.3 1区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-10-18 DOI: 10.1016/j.jcat.2026.117241
Boda Yang, Carlos Lizandara-Pueyo, Piyush Ingale, Ivana Jevtovikj, Reni Grauke, Stephan Schunk, Sungmin Kim, Huamin Wang, Johannes A. Lercher
{"title":"Impact of polyvinyl chloride on the hydrogenolysis of low-density polyethylene over supported transition metal catalysts","authors":"Boda Yang, Carlos Lizandara-Pueyo, Piyush Ingale, Ivana Jevtovikj, Reni Grauke, Stephan Schunk, Sungmin Kim, Huamin Wang, Johannes A. Lercher","doi":"10.1016/j.jcat.2026.117241","DOIUrl":"https://doi.org/10.1016/j.jcat.2026.117241","url":null,"abstract":"","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"39 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2026-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149232530","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
Structure–reactivity relationships in [Cp*Ru(MeCN)3][PF6]-catalyzed anti- and syn-selective hydrosilylation of internal alkynes and 1,3-diynes [Cp*Ru(MeCN)3][PF6]催化内炔和1,3-二炔反选择性和同选择性硅氢化反应的结构-反应关系
IF 7.3 1区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-10-01 DOI: 10.1016/j.jcat.2026.117229
Konrad Stęsik,Kinga Stefanowska,Jędrzej Walkowiak,Adrian Franczyk
{"title":"Structure–reactivity relationships in [Cp*Ru(MeCN)3][PF6]-catalyzed anti- and syn-selective hydrosilylation of internal alkynes and 1,3-diynes","authors":"Konrad Stęsik,Kinga Stefanowska,Jędrzej Walkowiak,Adrian Franczyk","doi":"10.1016/j.jcat.2026.117229","DOIUrl":"https://doi.org/10.1016/j.jcat.2026.117229","url":null,"abstract":"","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"9 1","pages":"117229"},"PeriodicalIF":7.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092080","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
Simple donor functionalization in D-A type conjugated polymers for improved photocatalytic H2O2 production activity under visible light D-A型共轭聚合物的简单给体功能化提高可见光下光催化生产H2O2的活性
IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-04-01 Epub Date: 2026-02-09 DOI: 10.1016/j.jcat.2026.116756
Changzhi Han , Tianci Chen , Shibo Lv , Jingwen Pan , Sihui Xiang , Jia-Xing Jiang
Anthraquinone (AQ) based organic conjugated polymers are promising photocatalysts for H2O2 photosynthesis from O2 and H2O, since the AQ unit with strong electron withdrawing ability can not only promote the charge separation but also act as redox active center to generate H2O2 via oxygen reduction reaction (ORR). Herein, three novel donor–acceptor type organic polymers are reported to elucidate the influence of simple donor functionalization on charge dynamics and ORR activity. Compared to biphenyl donor without functionalized group, acetylene functionalized diphenylacetylene donor and diacetylene functionalized 1,4-diphenylbutadiyne donor show reduced twisted angles between adjacent benzene rings and increased coplanarity of polymer chains, which promotes the charge transfer and separation along the polymer chains. Besides, the presence of diacetylene group in donor extends the π conjugation and broadens the light absorption range of DPB-AQ. Benefiting from the donor–acceptor structure, broad absorption range of visible light, upgraded charge transfer and separation ability, DPB-AQ exhibits a higher photocatalytic H2O2 yield of 7.8 mmol h−1 g−1 than BPH-AQ (1.0 mmol h−1 g−1) and DPA-AQ (3.8 mmol h−1 g−1) in pure water without additives. This work highlights the critical role of simple donor functionalization in polymers for H2O2 photosynthesis from H2O and O2.
蒽醌(AQ)基有机共轭聚合物具有很强的吸电子能力,不仅能促进电荷分离,还能作为氧化还原活性中心通过氧还原反应(ORR)生成H2O2,是O2和H2O光合作用的光催化剂。本文报道了三种新的给体-受体型有机聚合物,以阐明简单给体功能化对电荷动力学和ORR活性的影响。与不含官能团的联苯给体相比,乙炔官能团化的二苯基乙炔和二乙炔官能团化的1,4-二苯基丁二炔给体相邻苯环之间的扭角减小,聚合物链的共平面度增大,促进了电荷沿聚合物链的转移和分离。此外,二乙炔基团的存在扩大了DPB-AQ的π共轭,扩大了其光吸收范围。在无添加剂的纯水条件下,DPB-AQ光催化H2O2产率为7.8 mmol h−1 g−1,高于BPH-AQ (1.0mmol h−1 g−1)和DPA-AQ (3.8mmol h−1 g−1)。这项工作强调了简单的供体功能化在聚合物中从H2O和O2进行H2O2光合作用的关键作用。
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引用次数: 0
Manganese-catalyzed transfer hydrogenation of indoles to indolines: reaction scope and mechanistic investigation 锰催化吲哚转移加氢制吲哚:反应范围及机理研究
IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-04-01 Epub Date: 2026-02-04 DOI: 10.1016/j.jcat.2026.116732
Ying Xu , Zihan Zhang , Yizhou Wang , Longfei Li , Ning Ma , Zheng Wang , Huiliang Li , Yanping Ma , Wen-Hua Sun
A family of new ligands (L1–L8) and non-pincer-type PN-Mn(I) complex Mn1 containing the imidazoline motif have been successfully employed for the transfer hydrogenation of N-unprotected indoles with H3NBH3 (AB) as the hydrogen source, giving high efficiencies (TON up to 7200) and good compatibility with functional groups, which surpasses the activity of most effective noble metal catalysts for this reaction. The reaction kinetics investigations, control experiments, and DFT computations highlighted that the central amido/amino-based bifunctional activation step employed a concerted N–H and B-H activation reaction pathway, and the hydride/proton-transfer process is the rate-determining step. More importantly, a proposed catalytic cycle involves an outer-sphere pathway for the reduction of the isomerized CN bond rather than the CC bond in the indole. Furthermore, this catalytic protocol provides a convenient and efficient method for the synthesis of a wide variety of indolines (26 examples) and saturated N-heterocycles such as tetrahydroberberine (2 examples).
一类新的配体(L1-L8)和含有咪唑啉基的非钳型PN-Mn(I)配合物Mn1以H3NBH3 (AB)为氢源,成功地用于n-无保护的吲哚的转移加氢反应,具有很高的效率(TON高达7200)和与官能团的良好相容性,其活性超过了大多数有效的贵金属催化剂。反应动力学研究、对照实验和DFT计算表明,中心氨基/氨基双功能活化步骤采用协同的N-H和B-H活化反应途径,氢化物/质子转移过程是速率决定步骤。更重要的是,所提出的催化循环涉及一个外球途径,用于还原吲哚中的异构化CN键而不是CC键。此外,该催化方案为多种吲哚类化合物(26例)和饱和n -杂环化合物如四氢小檗碱(2例)的合成提供了一种方便高效的方法。
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引用次数: 0
Carbonylation catalysis of aryl halides through active-site engineering 活性位点工程催化芳基卤化物羰基化
IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-04-01 Epub Date: 2026-02-05 DOI: 10.1016/j.jcat.2026.116733
Arjun Neyyathala , Felix Jung , Claus Feldmann , Simon Barth , Jan-Dierk Grunwaldt , Ivana Jevtovikj , Stephan A. Schunk , Paolo Dolcet , Silvia Gross , Schirin Hanf
Crystalline palladium phosphide nanoparticles supported on silica (Pd3P/SiO2, 5 wt% Pd) are explored as catalysts for the alkoxycarbonylation of lignin-derived aromatic synthons, using model aryl halides as representative substrates. The detailed characterization by PXRD, HAADF-STEM, HRTEM, EDX, ICP-AES, XPS, CO-DRIFTS, and CO chemisorption confirmed the formation of the Pd3P phase with uniform nanoparticle size distribution. The catalytic performance was evaluated in a three-phase reaction system comprising a CO gas atmosphere, a liquid phase containing the solvent and substrate and a solid catalyst. The incorporation of phosphorus into the palladium lattice resulted in a more than two-fold enhancement in catalytic activity compared to conventional Pd-based heterogeneous catalysts. The Pd3P/SiO2 catalyst also outperformed several reported heterogeneous and commonly used homogeneous catalysts. This enhanced reactivity is attributed to the electronic and geometric effects introduced by phosphorus, which generate highly active, spatially-isolated Pd sites. These findings demonstrate the potential of Pd–P phase engineering for the design of the next-generation of carbonylation catalysts.
研究了二氧化硅负载的结晶磷化钯纳米颗粒(Pd3P/SiO2, 5 wt% Pd)作为木质素衍生芳香族合成物烷氧羰基化的催化剂,以模拟芳基卤化物为代表底物。通过PXRD、HAADF-STEM、HRTEM、EDX、ICP-AES、XPS、CO- drifts和CO化学吸附等详细表征,证实了Pd3P相的形成,具有均匀的纳米粒度分布。在一个由一氧化碳气体气氛、含有溶剂和底物的液相和固体催化剂组成的三相反应体系中评估了催化性能。与传统的钯基非均相体系相比,磷掺入钯晶格导致催化活性提高了两倍以上。Pd3P/SiO2催化剂的性能也优于几种已报道的多相和常用的均相催化剂。这种增强的反应性归因于磷引入的电子和几何效应,它们产生了高活性的、空间隔离的Pd位点。这些发现证明了Pd-P相工程在设计下一代羰基化催化剂方面的潜力。
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引用次数: 0
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Journal of Catalysis
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