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Acid gas valorization through a carbonyl sulfide (COS) intermediate over Na-containing FAU and LTA zeolites 通过羰基硫化物(COS)中间体在含na的FAU和LTA沸石上进行酸性气体增值
IF 5.3 2区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-15 Epub Date: 2025-12-21 DOI: 10.1016/j.cattod.2025.115660
Syeda Rabia Batool , Marco Fabbiani , Alexey Novikov , Raman Ghassemi , Soroush Zareghorbaei , Jeroen Lauwaert , Ludovic Pinard , Helene Retot , Joris W. Thybaut , Valentin Valtchev
A promising route for the valorization of acid gas (CO₂ and H₂S) components involves their simultaneous transformation into carbon monoxide and sulfur, through carbonyl sulfide (COS) intermediate. In this work, we systematically explore the catalytic performance of 13X and 4 A for COS formation under varying conditions of temperature, acid gas partial pressure, and zeolite hydration state. H2S, CO2, and COS breakthrough experiments at 45 °C reveal that the capacities of all three molecules are higher for 13X than for 4 A. Thermal gravimetry on hydrated zeolites specifies water contents of 13.1 and 12.0 mmol/g for 13X and 4 A, respectively. COS yield is highest at 100 °C, showing temperature dependence in the case of 13X; in contrast, 4 A retains more than 70 % of its maximum activity over an extended range of temperatures. An increase in acid gas partial pressure from 0.2 to 0.8 bar gradually increases the total COS in 13X, whereas the activity of 4 A remains constant. Likewise, COS formation increases with decreasing zeolite hydration; threshold-dependent in 13X but progressive and relatively less pronounced in 4 A. Both zeolites, independent of conditions, undergo a decline in COS formation over time due to the water-induced inhibition of active sites, attributed to poisoning. While activity in 4 A decays rapidly, 13X exhibits a more gradual decay, corresponding to the inhibitory effect of the produced water being less pronounced in 13X than in 4 A. This reduces competitive adsorption on active sites and mitigates site blockage in 13X, which in turn preserves catalytic performance over time, indicating that 13X is more sensitive to changing conditions than 4 A. An optimum operating window identified for the two materials can help reduce the energy required for the industrial conversion of acid gas and subsequent catalyst regeneration. This corresponds to reaction at 120 °C and 250 °C and the regeneration at 250 °C and 300 °C for 13X and 4 A, respectively.
酸性气体(CO₂和H₂S)组分的有希望的增值途径是通过羰基硫化物(COS)中间体将它们同时转化为一氧化碳和硫。在这项工作中,我们系统地探索了13X和4 A在不同温度、酸性气体分压和沸石水化状态下对COS形成的催化性能。在45 °C下进行的H2S, CO2和COS突破性实验表明,13X的这三种分子的容量都高于4 A。水合沸石的热重测定表明,13X和4 A的水含量分别为13.1和12.0 mmol/g。COS产率在100 °C时最高,在13X的情况下表现出温度依赖性;相比之下,4 A在更大的温度范围内保持了超过70% %的最大活性。随着酸性气体分压从0.2 ~ 0.8 bar的增加,13X的总COS逐渐增加,而4 A的活性保持不变。同样,随着沸石水化程度的降低,COS的形成也增加;13X的阈值依赖性,但4的进行性和相对不明显 A。随着时间的推移,这两种沸石(与条件无关)由于水诱导的活性位点的抑制而导致COS的形成下降,这归因于中毒。虽然4 A的活性衰减迅速,但13X的衰减更为缓慢,这与13X对产出水的抑制作用不如4 A明显相对应。这减少了活性位点上的竞争性吸附,减轻了13X的位点堵塞,从而随着时间的推移保持了催化性能,这表明13X对变化的条件比4 A更敏感。为这两种材料确定的最佳操作窗口可以帮助减少酸性气体的工业转化和随后的催化剂再生所需的能量。这对应于13X和4 A分别在120 °C和250 °C下的反应和250 °C和300 °C下的再生。
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引用次数: 0
A facile synthesis of α-phase palladium hydride ultrafine nanoparticles for accelerated formic acid electrooxidation α-相氢化钯纳米颗粒加速甲酸电氧化的制备
IF 5.3 2区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-15 Epub Date: 2026-01-08 DOI: 10.1016/j.cattod.2026.115683
Xinxin Tian , Chenyu Lv , Qinqin Mao , Peizhu Xu , Lixin Li , Xinhu Liang , Jun Li , Lili Han
Direct formic acid fuel cells (DFAFCs) have attracted considerable attention due to their high energy density and environmental benefits; however, their commercial application is hindered by the low activity, poor stability, and CO poisoning susceptibility of conventional Pd-based anode catalysts. In this study, we develop a facile and green aqueous synthesis strategy for fabricating ultrafine α-phase palladium hydride nanoparticles supported on carbon (α-PdH/C) through a combination of sonochemical and wet chemical reduction methods. The as-prepared α-PdH/C catalyst exhibits a uniform particle size of 3.62 ± 0.17 nm and a high electrochemical surface area of 131.28 m2 g‒1. It achieves a superior mass activity of 3.68 A mg‒1 for the formic acid oxidation reaction (FAOR), which is 3.35 times higher than that of Pd/C, along with significantly enhanced durability, showing negligible activity decay after 1000 cycles. In situ spectroscopic studies reveal that the FAOR reaction follows the formate pathways with negligible CO generation, a behavior attributed to the tensile strain induced by interstitial hydrogen atoms. This work provides an efficient Pd-based catalyst with remarkable performance and offers new insights into the design of advanced anodic electrocatalysts for DFAFCs.
直接甲酸燃料电池(dafcs)因其高能量密度和环境效益而受到广泛关注;然而,传统的钯基阳极催化剂活性低、稳定性差、CO中毒易感性等问题阻碍了它们的商业应用。在这项研究中,我们开发了一种简单、绿色的水合成策略,通过声化学和湿化学还原相结合的方法,制备了碳负载的超细α-相氢化钯纳米颗粒(α-PdH/C)。制备的α-PdH/C催化剂粒径均匀,为3.62 ±0.17 nm,电化学表面积高达131.28 m2 g-1。在甲酸氧化反应(FAOR)中,它的质量活性达到3.68 a mg-1,是Pd/C的3.35倍,并且耐久性显著提高,1000次循环后活性衰减可以忽略。原位光谱研究表明,FAOR反应遵循甲酸途径,CO的产生可以忽略,这一行为归因于间隙氢原子引起的拉伸应变。本研究提供了一种高效性能优异的pd基催化剂,为dafcs的先进阳极电催化剂的设计提供了新的见解。
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引用次数: 0
Upcycling plastic waste into polymeric composites with multani mitti for sustainable photodegradation of methylene blue: A comparative study with ZnO and Pzc evaluation 将塑料垃圾升级为聚合物复合材料用于亚甲基蓝的可持续光降解:氧化锌和Pzc评价的比较研究
IF 5.3 2区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-15 Epub Date: 2026-01-03 DOI: 10.1016/j.cattod.2026.115678
Agrima Singh , Megha Vijay , Deepa Sharma , Purnima Jain , Sapana Jadoun , Nirmala Kumari Jangid
The dual crises of plastic waste accumulation and wastewater contamination by toxic dyes demand sustainable, low-cost solutions. In this study, a plastic waste-derived polymeric composite, incorporating Multani Mitti (PWPA-MM), was fabricated through a simple one-step process and evaluated against a conventional ZnO photocatalyst for the photodegradation of the toxic dye Methylene Blue (MB). The PWPA-MM achieved 99.8 % dye removal at neutral pH (7) within 105 min, outperforming ZnO (89.56 % under identical conditions), with a degradation rate constant nearly 1.5 times higher. The FESEM confirmed its porous morphology, negative surface charge (-28.1 mV zeta potential), and a reduced band gap of 2.52 eV, which together enhanced charge separation and reactive species generation. Significantly, PWPA-MM reduced COD and BOD by more than 90 %, demonstrating its real wastewater treatment potential. Unlike conventional nanomaterials, this composite provides a circular economy pathway by valorising non-biodegradable plastic waste into a functional photocatalyst support. The findings establish PWPA-MM as a cost-effective and eco-friendly alternative to metal oxide nanomaterials, offering scalability and practical applications in industrial dye effluent treatment while addressing plastic waste management challenges simultaneously.
塑料废物堆积和有毒染料污染废水的双重危机需要可持续的、低成本的解决方案。在本研究中,通过简单的一步工艺制备了含有Multani Mitti (PWPA-MM)的塑料废物衍生聚合物复合材料,并与传统ZnO光催化剂进行了光降解有毒染料亚甲基蓝(MB)的评价。在中性pH(7)下,在105 min内,PWPA-MM的去除率达到99.8% %,优于相同条件下的ZnO(89.56 %),降解速率常数高出近1.5倍。FESEM证实了其多孔形态,负表面电荷(-28.1 mV zeta电位)和减小带隙(2.52 eV),共同促进了电荷分离和反应物质的产生。值得注意的是,PWPA-MM降低了COD和BOD超过90% %,显示了其真正的废水处理潜力。与传统的纳米材料不同,这种复合材料通过将不可生物降解的塑料废物转化为功能性光催化剂载体,提供了一种循环经济途径。研究结果表明,PWPA-MM是一种具有成本效益和环保的金属氧化物纳米材料替代品,在工业染料废水处理中提供可扩展性和实际应用,同时解决塑料废物管理挑战。
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引用次数: 0
Recent progress of advanced Co3O4-based materials for electrocatalytic oxygen evolution reaction in acid 先进co3o4基酸电催化析氧材料研究进展
IF 5.3 2区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-15 Epub Date: 2025-12-19 DOI: 10.1016/j.cattod.2025.115659
Zhe Wang, Yanwen Niu, Kaiyang Zhang, Rui Yao, Jinping Li, Guang Liu
Electrocatalytic water splitting provides a promising approach to produce high-purity hydrogen. Nevertheless, the overall efficiency scalability of water electrolysis is severely constrained by the slow kinetics of the oxygen evolution process.Developing high-efficiency, durable and low-cost OER(oxygen evolution reaction) catalysts is therefore essential. Materials based on spinel Co3O4 have garnered a lot of interest as potential substitutes for rare Ir- and Ru-based oxides, owing to their tunable electronic structure, notable OER activity in acidic media, and the earth abundance of cobalt. This paper first reviews the research progress on Co₃O₄-based acidic OER electrocatalysts, three OER mechanisms have been summarized. It then highlights various modification strategies such as noble and non-noble metal doping, morphology control, reaction pathway regulation, heterostructure construction, and single-atom catalysis. Subsequently, the OER performance of Co₃O₄-based electrocatalysts was comparatively evaluated. Finally, current challenges and future research toward high-performance Co3O4-based acidic OER electrocatalysts are outlined.
电催化水裂解是制备高纯度氢的一种很有前途的方法。然而,水电解的整体效率可扩展性受到析氧过程缓慢动力学的严重限制。因此,开发高效、耐用和低成本的OER(析氧反应)催化剂至关重要。基于尖晶石Co3O4的材料由于其可调谐的电子结构,在酸性介质中显着的OER活性以及钴的地球丰度而成为稀有的Ir和ru基氧化物的潜在替代品,引起了人们的极大兴趣。本文首先综述了Co₃O₄酸性OER电催化剂的研究进展,综述了三种OER机理。然后重点介绍了各种修饰策略,如贵金属和非贵金属掺杂,形态控制,反应途径调节,异质结构构建和单原子催化。随后,比较评价了Co₃O₄基电催化剂的OER性能。最后,对高性能co3o4基酸性OER电催化剂面临的挑战和未来的研究方向进行了展望。
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引用次数: 0
20th Japan-Korea Symposium on Catalysis 第20届日韩催化研讨会
IF 5.3 2区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-15 Epub Date: 2025-12-24 DOI: 10.1016/j.cattod.2025.115673
Masahiro Sadakane , Hyun-Seog Roh , Mikihiro Nomura
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引用次数: 0
Comparative study of hierarchical and nanosized SAPO-34 catalysts in methanol to olefins 分级与纳米级SAPO-34甲醇制烯烃催化剂的比较研究
IF 5.3 2区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-15 Epub Date: 2025-12-23 DOI: 10.1016/j.cattod.2025.115671
Rui Feng , Wei Wang , Junchao Luo , Tianbo Li , Xiaoyan Hu , Xinlong Yan , Shijian Lu
This study presents a comparative investigation of hierarchical and nanosized SAPO-34 catalysts for methanol-to-olefins (MTO) conversion. Hierarchical SAPO-34 (SP-Hx) was synthesized using PEG-4000 as a mesopore template, while nanosized SAPO-34 (SP-Nx) was prepared via a seed-assisted method. Characterization revealed that SP-H2 exhibited a hierarchical pore structure with enhanced external surface area (84 m2·g−1) and mesopore volume (0.35 cm3·g−1), whereas SP-N3 demonstrated reduced crystallite size of approximately 700 nm and higher acid site density. Catalytic tests showed that SP-N3 achieved the longest lifetime (625 min), a 2.2-fold increase over conventional SP-0 (275 min), attributed to its optimized acidity and shortened diffusion pathways. Hierarchical SP-H2 also exhibited improved stability (365 min) due to increased coke storage capacity. Coke analysis indicated that pore blockage by polycyclic aromatic hydrocarbons (PAHs) was the primary deactivation mechanism. These findings highlight the potential of nano-structuring and hierarchical design to enhance MTO catalyst performance.
本研究对甲醇制烯烃(MTO)的分级催化剂和纳米级催化剂SAPO-34进行了比较研究。以PEG-4000为介孔模板合成了分级SAPO-34 (SP-Hx),采用种子辅助法制备了纳米SAPO-34 (SP-Nx)。表征结果表明,SP-H2具有分层孔隙结构,外表面积增大(84 m2·g−1),介孔体积增大(0.35 cm3·g−1),而SP-N3晶粒尺寸减小,约为700 nm,酸位密度增大。催化测试表明,SP-N3获得了最长的寿命(625 min),比常规SP-0(275 min)增加了2.2倍,这归功于其优化的酸性和缩短的扩散途径。分级SP-H2也表现出了更好的稳定性(365 min),因为增加了焦炭储存能力。焦炭分析表明,多环芳烃(PAHs)堵塞孔隙是主要失活机制。这些发现突出了纳米结构和分层设计在提高MTO催化剂性能方面的潜力。
{"title":"Comparative study of hierarchical and nanosized SAPO-34 catalysts in methanol to olefins","authors":"Rui Feng ,&nbsp;Wei Wang ,&nbsp;Junchao Luo ,&nbsp;Tianbo Li ,&nbsp;Xiaoyan Hu ,&nbsp;Xinlong Yan ,&nbsp;Shijian Lu","doi":"10.1016/j.cattod.2025.115671","DOIUrl":"10.1016/j.cattod.2025.115671","url":null,"abstract":"<div><div>This study presents a comparative investigation of hierarchical and nanosized SAPO-34 catalysts for methanol-to-olefins (MTO) conversion. Hierarchical SAPO-34 (SP-H<em>x</em>) was synthesized using PEG-4000 as a mesopore template, while nanosized SAPO-34 (SP-N<em>x</em>) was prepared via a seed-assisted method. Characterization revealed that SP-H2 exhibited a hierarchical pore structure with enhanced external surface area (84 m<sup>2</sup>·g<sup>−1</sup>) and mesopore volume (0.35 cm<sup>3</sup>·g<sup>−1</sup>), whereas SP-N3 demonstrated reduced crystallite size of approximately 700 nm and higher acid site density. Catalytic tests showed that SP-N3 achieved the longest lifetime (625 min), a 2.2-fold increase over conventional SP-0 (275 min), attributed to its optimized acidity and shortened diffusion pathways. Hierarchical SP-H2 also exhibited improved stability (365 min) due to increased coke storage capacity. Coke analysis indicated that pore blockage by polycyclic aromatic hydrocarbons (PAHs) was the primary deactivation mechanism. These findings highlight the potential of nano-structuring and hierarchical design to enhance MTO catalyst performance.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"466 ","pages":"Article 115671"},"PeriodicalIF":5.3,"publicationDate":"2026-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145838675","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Micro-mixer combined with Au/TS-1 catalyst for improving the efficiency and safety of gas-phase propylene epoxidation Au/TS-1催化剂复合微混合器提高气相丙烯环氧化效率和安全性
IF 5.3 2区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-15 Epub Date: 2025-12-21 DOI: 10.1016/j.cattod.2025.115661
Yupeng Tian , Yujia Liu , Shoutao Ma , Wei Xu , Chenyang Zhao , Bing Sun
This study introduces a heart-like micromixer reactor and Au/TS-1 catalyst to address the dual challenges of safety and efficiency in gas-phase propylene epoxidation using H2 and O2. Conventional methods face inherent explosion risks and rapid catalyst deactivation due to sintering and coking. The microreactor architecture achieves over 99 % flame-quenching efficiency via sub-millisecond radical suppression and enhanced heat transfer, enabling safe operation with minimal inert gas dilution (N2 < 70 vol%). Coupled with alkali-promoted Au/TS-1 catalysts, the system sustains > 90 % propylene oxide (PO) selectivity for 500 h, outperforming static mixers where activity halved within 100 h. This work pioneers a reactor-catalyst co-design strategy, decoupling safety constraints from reaction efficiency, and establishes a scalable platform for sustainable PO synthesis. Besides, the critical gaps in industrial-scale implementation of explosive gas-phase reactions is bridged.
本研究介绍了一种类似心脏的微混合器反应器和Au/TS-1催化剂,以解决H2和O2气相环氧化丙烯的安全性和效率的双重挑战。传统的方法存在固有的爆炸风险,并且由于烧结和焦化导致催化剂快速失活。微反应器结构通过亚毫秒级的自由基抑制和增强的传热,实现了99% %以上的火焰熄灭效率,在最小的惰性气体稀释(N2 < 70 vol%)下实现了安全运行。与碱促进的Au/TS-1催化剂相结合,该体系在500 h内保持了>; 90%的环氧丙烷(PO)选择性,优于静态混合器,后者的活性在100 h内减半。这项工作开创了反应器-催化剂协同设计策略,将安全约束与反应效率脱钩,并建立了可扩展的可持续PO合成平台。此外,还填补了爆炸性气相反应工业规模实施的关键空白。
{"title":"Micro-mixer combined with Au/TS-1 catalyst for improving the efficiency and safety of gas-phase propylene epoxidation","authors":"Yupeng Tian ,&nbsp;Yujia Liu ,&nbsp;Shoutao Ma ,&nbsp;Wei Xu ,&nbsp;Chenyang Zhao ,&nbsp;Bing Sun","doi":"10.1016/j.cattod.2025.115661","DOIUrl":"10.1016/j.cattod.2025.115661","url":null,"abstract":"<div><div>This study introduces a heart-like micromixer reactor and Au/TS-1 catalyst to address the dual challenges of safety and efficiency in gas-phase propylene epoxidation using H<sub>2</sub> and O<sub>2</sub>. Conventional methods face inherent explosion risks and rapid catalyst deactivation due to sintering and coking. The microreactor architecture achieves over 99 % flame-quenching efficiency via sub-millisecond radical suppression and enhanced heat transfer, enabling safe operation with minimal inert gas dilution (N<sub>2</sub> &lt; 70 vol%). Coupled with alkali-promoted Au/TS-1 catalysts, the system sustains &gt; 90 % propylene oxide (PO) selectivity for 500 h, outperforming static mixers where activity halved within 100 h. This work pioneers a reactor-catalyst co-design strategy, decoupling safety constraints from reaction efficiency, and establishes a scalable platform for sustainable PO synthesis. Besides, the critical gaps in industrial-scale implementation of explosive gas-phase reactions is bridged.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"466 ","pages":"Article 115661"},"PeriodicalIF":5.3,"publicationDate":"2026-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145838677","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Effect of sodium precursors on Na-Ru/Al2O3 dual function materials for integrated CO2 capture and methanation 钠前驱体对Na-Ru/Al2O3双功能材料CO2捕集与甲烷化的影响
IF 5.3 2区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-15 Epub Date: 2025-12-23 DOI: 10.1016/j.cattod.2025.115668
Eun Ji Kim , Dong Chan Park , Sang Hun Choi , Sein Hwang , Do Heui Kim , Inhak Song
The influence of alkali metal precursor on Dual-Function Materials (DFMs) for integrated CO2 capture and methanation has not been thoroughly explored. This study systematically investigated the effect of sodium carbonate and sodium nitrate precursors on Na-Ru/Al2O3 DFM performance. The two precursors exhibited markedly different thermal decomposition behaviors. After calcination at 400 °C, carbonate precursors retained 3.7 % carbon while nitrate precursors underwent complete decomposition. This difference proved critical for catalyst performance. Catalysts derived from sodium carbonate precursors (Na(C)-Ru/Al) produced 1.9 times less methane than the sodium nitrate-derived catalysts (Na(N)-Ru/Al). They also showed delayed methane formation with substantial CO2 detected upon hydrogen injection for methanation. Even after substantial decomposition of carbonate precursor at 600 °C it exhibited low activity. Initial methane formation rates of Na(C)-Ru/Al600 sample reached only 0.56 μmol/min·gcat compared to 1.52 μmol/min·gcat for the nitrate-based system, Na(N)-Ru/Al600. XRD analysis revealed progressive sodium aluminate formation upon carbonate decomposition, which likely contributed to the low methane productivity by hindering RuOx reduction. This structural transformation elevated RuOx reduction temperature from 148 °C (Ru/Al400_600 reference) to 223 °C. In contrast, nitrate-derived samples prevented this structural change and maintained optimal reduction of RuOx at 124 °C. The impact of calcination atmosphere on catalyst stability was also investigated by calcining Na(C)-Ru/Al samples under static air, CO2, O2, and N2 atmospheres. Notably, calcination under CO2 atmosphere prevented Ru volatilization and maintained optimal Na+ dispersion. In contrast, other atmospheres led to detrimental NaAlO2 formation, which is associated with catalytic performance.
碱金属前驱体对二氧化碳捕集与甲烷化双功能材料的影响尚未深入研究。系统研究了碳酸钠和硝酸钠前驱体对Na-Ru/Al2O3 DFM性能的影响。两种前驱体表现出明显不同的热分解行为。在400 °C煅烧后,碳酸盐前驱体保留了3.7 %的碳,而硝酸盐前驱体完全分解。这种差异对催化剂的性能至关重要。由碳酸钠衍生的催化剂(Na(C)-Ru/Al)产生的甲烷比由硝酸钠衍生的催化剂(Na(N)-Ru/Al)产生的甲烷少1.9倍。他们还发现甲烷形成延迟,在注入氢气进行甲烷化时检测到大量的二氧化碳。即使碳酸盐前驱体在600 °C时大量分解,其活性也很低。Na(N)-Ru/Al600样品的初始甲烷生成速率仅为0.56 μmol/min·gcat,而Na(N)-Ru/Al600样品的初始甲烷生成速率为1.52 μmol/min·gcat。XRD分析表明,碳酸盐岩分解过程中会逐渐形成铝酸钠,这可能阻碍了氧化还原,导致甲烷产率较低。这种结构转变将RuOx还原温度从148 °C (Ru/Al400_600参考)提高到223 °C。相比之下,硝酸盐衍生的样品阻止了这种结构变化,并在124 °C下保持了最佳的RuOx还原。通过在静态空气、CO2、O2和N2气氛下煅烧Na(C)-Ru/Al样品,考察了煅烧气氛对催化剂稳定性的影响。值得注意的是,在CO2气氛下煅烧可以阻止Ru的挥发,并保持最佳的Na+分散。相反,其他气氛导致有害的NaAlO2形成,这与催化性能有关。
{"title":"Effect of sodium precursors on Na-Ru/Al2O3 dual function materials for integrated CO2 capture and methanation","authors":"Eun Ji Kim ,&nbsp;Dong Chan Park ,&nbsp;Sang Hun Choi ,&nbsp;Sein Hwang ,&nbsp;Do Heui Kim ,&nbsp;Inhak Song","doi":"10.1016/j.cattod.2025.115668","DOIUrl":"10.1016/j.cattod.2025.115668","url":null,"abstract":"<div><div>The influence of alkali metal precursor on Dual-Function Materials (DFMs) for integrated CO<sub>2</sub> capture and methanation has not been thoroughly explored. This study systematically investigated the effect of sodium carbonate and sodium nitrate precursors on Na-Ru/Al<sub>2</sub>O<sub>3</sub> DFM performance. The two precursors exhibited markedly different thermal decomposition behaviors. After calcination at 400 °C, carbonate precursors retained 3.7 % carbon while nitrate precursors underwent complete decomposition. This difference proved critical for catalyst performance. Catalysts derived from sodium carbonate precursors (Na(C)-Ru/Al) produced 1.9 times less methane than the sodium nitrate-derived catalysts (Na(N)-Ru/Al). They also showed delayed methane formation with substantial CO<sub>2</sub> detected upon hydrogen injection for methanation. Even after substantial decomposition of carbonate precursor at 600 °C it exhibited low activity. Initial methane formation rates of Na(C)-Ru/Al600 sample reached only 0.56 μmol/min·g<sub>cat</sub> compared to 1.52 μmol/min·g<sub>cat</sub> for the nitrate-based system, Na(N)-Ru/Al600. XRD analysis revealed progressive sodium aluminate formation upon carbonate decomposition, which likely contributed to the low methane productivity by hindering RuO<sub>x</sub> reduction. This structural transformation elevated RuO<sub>x</sub> reduction temperature from 148 °C (Ru/Al400_600 reference) to 223 °C. In contrast, nitrate-derived samples prevented this structural change and maintained optimal reduction of RuO<sub>x</sub> at 124 °C. The impact of calcination atmosphere on catalyst stability was also investigated by calcining Na(C)-Ru/Al samples under static air, CO<sub>2</sub>, O<sub>2</sub>, and N<sub>2</sub> atmospheres. Notably, calcination under CO<sub>2</sub> atmosphere prevented Ru volatilization and maintained optimal Na<sup>+</sup> dispersion. In contrast, other atmospheres led to detrimental NaAlO<sub>2</sub> formation, which is associated with catalytic performance.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"466 ","pages":"Article 115668"},"PeriodicalIF":5.3,"publicationDate":"2026-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145838676","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
A new horizon in green synthesis for metal oxides: Dracaena reflexa-derived TiO₂ nanoparticles for photocatalytic activity and antibacterial application 绿色合成金属氧化物的新领域:龙血树反射衍生的二氧化钛纳米粒子的光催化活性和抗菌应用
IF 5.3 2区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-15 Epub Date: 2026-01-03 DOI: 10.1016/j.cattod.2026.115679
Harshita Shrivastav , Harpreet Kaur , Sanjeev Kumar , Dharmesh Sur , Shima Sadaf , Ramandeep Kaur , Chandra Kumar , Payal Patial , Mohammed Awad , Mir Waqas Alam
This study introduces a novel, sustainable approach for the synthesis of Titanium dioxide nanoparticles (TiO₂ NPs), utilizing Dracaena reflexa (DR) leaf extract as a biogenic source of reducing and capping agents, for the first time. X-ray diffraction (XRD) analysis confirmed the anatase phase with an average crystallite size of 8.89 nm. UV-Vis spectroscopy revealed a strong absorption peak at 250 nm and an optical band gap of 3.63 eV, which suggested the material’s potential for UV-driven photocatalytic applications. Gas chromatography-mass spectra (GC-MS) of DR plant extract have revealed the presence of various phytochemical compounds and their class. Fourier-transform infrared (FTIR) analysis showed interactions between the plant extract and TiO₂, with phytochemicals playing a key role in nanoparticle formation. Field emission scanning electron microscopy (FESEM) images revealed spherical nanoparticles with minimal agglomeration. Energy-dispersive X-ray spectroscopy (EDS) and elemental mapping confirmed the presence of Ti and O. Thermogravimetric analysis (TGA) showed that the mass stabilized above 550 °C, with nearly 89 wt% retained at 800 °C. Brunauer-Emmett-Teller (BET) surface area analysis indicated a high specific surface area of 250.606 m²/g, ideal for photocatalytic applications. This exceptionally high surface area of DR/TiO₂ NPs represents a remarkable achievement. The present study demonstrates an exceptional 99 % degradation of Methyl Orange (MO) dye within just 90 min under UV light using DR/TiO₂ as a photocatalyst. Additionally, the order of influence of scavengers on the photodegradation mechanism is found to be h+ > •OH > O₂⁻•. The complete degradation mechanism is elucidated by GC-MS analysis of the dye. DR/TiO₂ NPs exhibited superior antibacterial activity against S. aureus and E. coli, with clearly defined inhibition zones increasing in size at higher concentrations. Thus, the present results depicted the successful green synthesis of TiO₂ NPs, making them suitable for environmental remediation, wastewater treatment, and biomedical applications.
本研究首次采用龙血树(Dracaena reflexa, DR)叶提取物作为还原剂和封盖剂的生物源,合成二氧化钛纳米颗粒(TiO₂NPs)。x射线衍射(XRD)分析证实为锐钛矿相,平均晶粒尺寸为8.89 nm。紫外可见光谱显示,该材料在250 nm处有很强的吸收峰,光学带隙为3.63 eV,这表明该材料具有紫外驱动光催化应用的潜力。通过气相色谱-质谱(GC-MS)分析,发现了多种植物化学成分及其种类。傅里叶红外(FTIR)分析表明,植物提取物与tio2之间存在相互作用,植物化学物质在纳米颗粒的形成中起关键作用。场发射扫描电镜(FESEM)图像显示球形纳米颗粒具有最小的团聚。能量色散x射线能谱(EDS)和元素图证实了Ti和o的存在,热重分析(TGA)表明,质量稳定在550°C以上,800°C时保留近89 wt%。brunauer - emmet - teller (BET)表面积分析表明,该材料的高比表面积为250.606 m²/g,是光催化应用的理想材料。DR/ tio2nps的高表面积是一项了不起的成就。本研究表明,在紫外光下,使用DR/TiO 2作为光催化剂,甲基橙(MO)染料在90 min内的降解率为99% %。此外,发现清除剂对光降解机制的影响顺序为h+ >;•OH >; O₂⁻•。通过气相色谱-质谱分析阐明了染料的完全降解机理。DR/TiO 2 NPs对金黄色葡萄球菌和大肠杆菌具有良好的抑菌活性,抑菌带清晰,浓度越高抑菌带的大小越大。因此,本研究结果描述了tio2nps的成功绿色合成,使其适用于环境修复,废水处理和生物医学应用。
{"title":"A new horizon in green synthesis for metal oxides: Dracaena reflexa-derived TiO₂ nanoparticles for photocatalytic activity and antibacterial application","authors":"Harshita Shrivastav ,&nbsp;Harpreet Kaur ,&nbsp;Sanjeev Kumar ,&nbsp;Dharmesh Sur ,&nbsp;Shima Sadaf ,&nbsp;Ramandeep Kaur ,&nbsp;Chandra Kumar ,&nbsp;Payal Patial ,&nbsp;Mohammed Awad ,&nbsp;Mir Waqas Alam","doi":"10.1016/j.cattod.2026.115679","DOIUrl":"10.1016/j.cattod.2026.115679","url":null,"abstract":"<div><div>This study introduces a novel, sustainable approach for the synthesis of Titanium dioxide nanoparticles (TiO₂ NPs), utilizing <em>Dracaena reflexa</em> (<em>DR</em>) leaf extract as a biogenic source of reducing and capping agents, for the first time. X-ray diffraction (XRD) analysis confirmed the anatase phase with an average crystallite size of 8.89 nm. UV-Vis spectroscopy revealed a strong absorption peak at 250 nm and an optical band gap of 3.63 eV, which suggested the material’s potential for UV-driven photocatalytic applications. Gas chromatography-mass spectra (GC-MS) of <em>DR</em> plant extract have revealed the presence of various phytochemical compounds and their class. Fourier-transform infrared (FTIR) analysis showed interactions between the plant extract and TiO₂, with phytochemicals playing a key role in nanoparticle formation. Field emission scanning electron microscopy (FESEM) images revealed spherical nanoparticles with minimal agglomeration. Energy-dispersive X-ray spectroscopy (EDS) and elemental mapping confirmed the presence of Ti and O. Thermogravimetric analysis (TGA) showed that the mass stabilized above 550 °C, with nearly 89 wt% retained at 800 °C. Brunauer-Emmett-Teller (BET) surface area analysis indicated a high specific surface area of 250.606 m²/g, ideal for photocatalytic applications. This exceptionally high surface area of <em>DR</em>/TiO₂ NPs represents a remarkable achievement. The present study demonstrates an exceptional 99 % degradation of Methyl Orange (MO) dye within just 90 min under UV light using <em>DR</em>/TiO₂ as a photocatalyst. Additionally, the order of influence of scavengers on the photodegradation mechanism is found to be h<sup>+</sup> &gt; •OH &gt; O₂⁻•. The complete degradation mechanism is elucidated by GC-MS analysis of the dye. <em>DR</em>/TiO₂ NPs exhibited superior antibacterial activity against <em>S. aureus</em> and <em>E. coli</em>, with clearly defined inhibition zones increasing in size at higher concentrations. Thus, the present results depicted the successful green synthesis of TiO₂ NPs, making them suitable for environmental remediation, wastewater treatment, and biomedical applications.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"466 ","pages":"Article 115679"},"PeriodicalIF":5.3,"publicationDate":"2026-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145939929","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Recent advances in the preparation of 2,6-dimethylnaphthalene 2,6-二甲基萘的制备研究进展
IF 5.3 2区 化学 Q1 CHEMISTRY, APPLIED Pub Date : 2026-03-15 Epub Date: 2025-12-29 DOI: 10.1016/j.cattod.2025.115676
Guang-Rong Ding , Hua Xin , Ye Zhang , Kuan-Rong Xue , Sheng-Dong Yang , Yong-Gang Wang , Feng-Shou Xiao
Poly(ethylene naphthalate) (PEN) is a high-performance engineering polyester with critical applications in multiple fields such as precision packaging and aerospace systems. Nevertheless, its industrial-scale implementation remains constrained by the high production costs of its crucial precursor, 2,6-dimethylnaphthalene (2,6-DMN). This review has comprehensively summarized the preparation methods for 2,6-DMN, which are categorized into direct extraction and catalytic synthesis. Direct extraction achieved high-purity 2,6-DMN from coal/petroleum-derived oils via multi-stage purification cascades. Catalytic synthesis techniques are divided into four distinct pathways: (i) o-xylene alkenylation with butadiene, (ii) p-xylene/C4 olefin coupling, (iii) toluene acylation, and (iv) naphthalene (NAPH)/2-methylnaphthalene (2-MN) methylation. Among these, zeolite-catalyzed alkylation of NAPH/2-MN with methanol demonstrated compelling industrial potential due to its cost-effective feedstocks and simplified process. We further highlight mechanistic insights into alkylation pathways and reactant diffusion dynamics, which have driven intensive research into the design of zeolite catalysts, particularly the regulation of acidity and pore architecture to enhance shape-selectivity. Using representative zeolites (HZSM-5, HZSM-12, SAPO-11) as model systems, we critically evaluated structure-activity relationships in catalyst modification strategies, including acid site density modulation, mesoporosity introduction and surface passivation, along with their corresponding impact on methylation performance. Finally, four strategic research priorities are proposed to advance next-generation catalysts for scalable and economically sustainable 2,6-DMN production.
聚萘二甲酸乙酯(PEN)是一种高性能工程聚酯,在精密包装和航空航天系统等多个领域具有重要应用。然而,其工业规模的实施仍然受到其关键前体2,6-二甲基萘(2,6- dmn)的高生产成本的限制。综述了2,6- dmn的制备方法,主要分为直接萃取法和催化合成法。通过多级纯化级联,直接从煤/石油衍生油中提取高纯度的2,6- dmn。催化合成技术分为四种不同的途径:(i)邻二甲苯烯基化与丁二烯,(ii)对二甲苯/C4烯烃偶联,(iii)甲苯酰化,和(iv)萘(NAPH)/2-甲基萘(2-MN)甲基化。其中,沸石催化的NAPH/2-MN与甲醇的烷基化反应因其成本效益高和工艺简化而具有引人注目的工业潜力。我们进一步强调了对烷基化途径和反应物扩散动力学的机理见解,这推动了对沸石催化剂设计的深入研究,特别是对酸度和孔结构的调节,以提高形状选择性。以具有代表性的沸石(HZSM-5, HZSM-12, SAPO-11)为模型体系,我们批判性地评估了催化剂改性策略中的结构-活性关系,包括酸位密度调节,介孔引入和表面钝化,以及它们对甲基化性能的相应影响。最后,提出了四个战略研究重点,以推进下一代催化剂的可扩展和经济可持续的2,6- dmn生产。
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