Chem Catalysis最新文献_第9页

Ligands-regulated ∗CO adsorption on two-dimensional covalent organic framework promotes selective electrochemical CO2 conversion 配体调控的* CO在二维共价有机框架上的吸附促进了选择性的电化学CO2转化

IF 9.4

Chem Catalysis Pub Date : 2025-03-19 DOI: 10.1016/j.checat.2025.101325

Yuluo Shen, Jiyuan Liu, Guoshuai Shi, Chunlei Yang, Tingyu Lu, Mingwei Chang, Yijie Wu, Shuzhou Li, Dong-Jin Qian, Liming Zhang

{"title":"Ligands-regulated ∗CO adsorption on two-dimensional covalent organic framework promotes selective electrochemical CO2 conversion","authors":"Yuluo Shen, Jiyuan Liu, Guoshuai Shi, Chunlei Yang, Tingyu Lu, Mingwei Chang, Yijie Wu, Shuzhou Li, Dong-Jin Qian, Liming Zhang","doi":"10.1016/j.checat.2025.101325","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101325","url":null,"abstract":"Manipulating the adsorption/desorption of intermediates at active sites offers a promising strategy to direct specific electrocatalytic pathways. In high overpotential regimes, the desorption of ∗CO from active sites is a major limitation in electrochemical CO2-to-CO conversion, emphasizing the need to control ∗CO adsorption strength. Here, we report a series of well-defined amide-linked covalent organic frameworks (COFs) featuring alternating tetraaminophenylporphyrin and tetracarboxyphenylporphyrin building blocks, with M1 and M2 sites (M1/M2 = Co, Fe). Electrochemical tests and computational models reveal that the polar ligand framework plays a key role in regulating ∗CO adsorption, a conclusion supported by operando spectroelectrochemical measurements. Theoretical calculations attribute this regulation to the differing <math><mrow is=\"true\"><msub is=\"true\"><mi is=\"true\" mathvariant=\"normal\">d</mi><msup is=\"true\"><mi is=\"true\" mathvariant=\"normal\">z</mi><mn is=\"true\">2</mn></msup></msub></mrow></math> band centers of the transition metals, driven by intra-layer charge transfer from polar amine bonds. This work underscores the importance of polar ligands in optimizing intermediate adsorption and enhancing CO2 transformation efficiency.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"70 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143653996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dynamic kinetic resolution and dynamic kinetic asymmetric transformation of atropisomeric biaryls atroisomer biaryl的动态动力学拆分和动态动力学不对称转化

IF 9.4

Chem Catalysis Pub Date : 2025-03-18 DOI: 10.1016/j.checat.2025.101329

Jie Zhang, Xuanzhu Huo, Yidan Liu, Can Zhu

引用次数: 0

The advances in innovative amorphous noble-metal-based electrocatalysts 新型非晶贵金属基电催化剂的研究进展

IF 9.4

Chem Catalysis Pub Date : 2025-03-18 DOI: 10.1016/j.checat.2025.101324

Xiaoyu Fan, Kexin Yin, Huiqing Wang, Jinlong Zheng, Jie Lin, Binbin Jia, Mingyuan Xu, Liqun Ye

引用次数: 0

Customizing biocatalysts by reducing ΔG‡: Integrating ground-state destabilization and transition-state stabilization 通过降低ΔG定制生物催化剂：整合基态不稳定和过渡态稳定

IF 9.4

Chem Catalysis Pub Date : 2025-03-17 DOI: 10.1016/j.checat.2025.101323

Xin Xu, Wanqing Wei, Yiwen Zhou, Jia Liu, Cong Gao, Guipeng Hu, Xiaomin Li, Jian Wen, Liming Liu, Jing Wu, Wei Song

{"title":"Customizing biocatalysts by reducing ΔG‡: Integrating ground-state destabilization and transition-state stabilization","authors":"Xin Xu, Wanqing Wei, Yiwen Zhou, Jia Liu, Cong Gao, Guipeng Hu, Xiaomin Li, Jian Wen, Liming Liu, Jing Wu, Wei Song","doi":"10.1016/j.checat.2025.101323","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101323","url":null,"abstract":"Enzymatic catalysts are increasingly recognized for their potential to revolutionize the chemical industry by enabling precise control of reaction pathways, reducing energy consumption, and minimizing waste, thereby offering exceptional selectivity and sustainability. Enzyme engineering, which focuses on modifying natural enzymes to meet industrial needs, plays a pivotal role in this transformation. A key objective of enzyme engineering is to lower the free energy barrier (ΔG‡). This review delves into computationally driven strategies designed to accomplish this objective. These strategies are classified into two distinct approaches: ground-state destabilization (GSD) and transition-state stabilization (TSS). For example, GSD may involve reshaping the hydrogen bonding network to elevate ground state energy, while TSS can stabilize the transition state by modulating local electric fields. GSD strategies involve modulating substrate-binding free energy to destabilize the ground state, reshaping hydrogen bonding networks, and refining binding conformations. TSS methods involve modulating proton and electron transfers, optimizing local electric fields, and modifying active sites based on transition-state models. Furthermore, this review contrasts GSD and TSS approaches, discussing their computational underpinnings, respective advantages, and limitations throughout the text to provide a comprehensive understanding of their applications. Finally, we explore technical challenges, the impact of emerging technologies, and the directions and trends of future research.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"39 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635654","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Unlocking redox-active reactivity of dearomatized pyridines with photochemistry toward meta-C–H functionalization of pyridines 用光化学技术开启脱芳烃吡啶的氧化还原活性反应，实现吡啶的元-C-H 功能化

IF 9.4

Chem Catalysis Pub Date : 2025-03-17 DOI: 10.1016/j.checat.2025.101326

Mingkai Yang, Mei Wang, Haiman Zhang, Shi Qin, Manzoor Zaman, Jiayu Luo, Shiping Zhan, Xu Wang, Cheng Zhang, Shengdong Wang, Hui Gao, Zhi Zhou, A. Stephen K. Hashmi, Wei Yi, Zhongyi Zeng

{"title":"Unlocking redox-active reactivity of dearomatized pyridines with photochemistry toward meta-C–H functionalization of pyridines","authors":"Mingkai Yang, Mei Wang, Haiman Zhang, Shi Qin, Manzoor Zaman, Jiayu Luo, Shiping Zhan, Xu Wang, Cheng Zhang, Shengdong Wang, Hui Gao, Zhi Zhou, A. Stephen K. Hashmi, Wei Yi, Zhongyi Zeng","doi":"10.1016/j.checat.2025.101326","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101326","url":null,"abstract":"Selective meta-C–H functionalization of pyridines is particularly attractive in synthetic and medicinal chemistry but remains largely underdeveloped due to their intrinsic electronic nature. Therefore, temporary dearomatization has gradually evolved as a powerful tool for this selective transformation. However, established methods all utilized dearomatized pyridine intermediates as redox-inert π-electron donors to react with ionic or radical-type electrophiles. Herein, the redox-active reactivity of dearomatized oxazino-pyridines is unlocked by photochemistry, providing a unified and modular platform for meta-C–H sulfonylation, sulfamoylation, and trifluoromethylation of pyridines. Integrated experimental and computational mechanistic studies revealed the concurrent generation of oxazino-pyridine radicals and sulfonyl radicals as well as their polarity-matched radical-radical couplings. This mild protocol features complete regiocontrol, remarkable functional group compatibility, and practical applicability in late-stage modification of bioactive molecules.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"55 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635657","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Will biohybrid or tandem CO2 electrolysis prevail? 生物混合或串联二氧化碳电解会流行吗？

IF 9.4

Chem Catalysis Pub Date : 2025-03-11 DOI: 10.1016/j.checat.2025.101322

Keoni Young, Sophie Kochanek, Gavin Silveira, Joshua Jack

引用次数: 0

Ensembled Ptδ+ species on Beta zeolites for efficient preferential oxidation of CO in H2 β沸石上的Ptδ+物质对CO在H2中的有效优先氧化

IF 9.4

Chem Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.checat.2025.101302

Jia Shen, Qian Xiang, Lichuan Song, Yake Lou, Jiajie Ye, Xiao Yang, Yanglong Guo, Wangcheng Zhan, Li Wang, Xiao-Ming Cao, Xuan Tang, Sheng Dai, Yun Guo

{"title":"Ensembled Ptδ+ species on Beta zeolites for efficient preferential oxidation of CO in H2","authors":"Jia Shen, Qian Xiang, Lichuan Song, Yake Lou, Jiajie Ye, Xiao Yang, Yanglong Guo, Wangcheng Zhan, Li Wang, Xiao-Ming Cao, Xuan Tang, Sheng Dai, Yun Guo","doi":"10.1016/j.checat.2025.101302","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101302","url":null,"abstract":"The preferential oxidation of CO in H2-rich environments (CO-PROX) is one of the most promising strategies for purifying H2. However, developing catalysts with low noble metal loadings that can effectively operate within a wide temperature range remains a significant challenge. Here, we synthesized ensembled Ptδ+ species on Beta zeolite (0.36 wt % Pt) through a reduction treatment. This catalyst achieved 100% CO conversion in CO-PROX across the temperature range of 25°C–220°C. The outstanding performance of this catalyst originates from the temperature-dependent dual mechanisms. Specifically, the ensembled Ptδ+ species weaken the adsorption strength of CO and enhance activation in O2 at elevated temperatures. Moreover, these Ptδ+ species play a crucial role in facilitating the adsorption and dissociation of H2 at lower temperatures, enabling it to react with O2 and form –OH species. These –OH species readily react with CO, overcoming the challenges associated with O2 activation.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"54 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143582552","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Durability of PGM catalyst MEAs of polymer electrolyte membrane fuel cells for heavy-duty vehicles 重型车用聚合物电解质膜燃料电池PGM催化剂MEAs耐久性研究

IF 9.4

Chem Catalysis Pub Date : 2025-03-07 DOI: 10.1016/j.checat.2025.101303

Guangqi Zhu, Qi Zhang, Chenzhao Li, Haoran Yu, David A. Cullen, Oana C. Marina, Zheng-Hua Li, David M. Wayne, Jian Xie

{"title":"Durability of PGM catalyst MEAs of polymer electrolyte membrane fuel cells for heavy-duty vehicles","authors":"Guangqi Zhu, Qi Zhang, Chenzhao Li, Haoran Yu, David A. Cullen, Oana C. Marina, Zheng-Hua Li, David M. Wayne, Jian Xie","doi":"10.1016/j.checat.2025.101303","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101303","url":null,"abstract":"Polymer electrolyte membrane fuel cells (PEMFCs) are promising power sources for heavy-duty vehicles (HDVs) owing to cleanliness and efficiency. However, the degradation of membrane electrode assemblies (MEAs) under HDV conditions remains a huge challenge. This work investigated MEA durability under HDV conditions using a US Department of Energy standard accelerated stress test for 180,000 cycles (equivalent to 1 million miles of HDV operation). Effects of catalyst Pt content on MEA durability were examined using homemade 30% Pt/C (H-Pt/C) and commercial 46% Pt/C (C-Pt/C) catalysts. Both MEAs experienced H2/air and H2/O2 performance loss over cycles. Analysis with scanning transmission electron microscopy, X-ray diffraction, inductively coupled plasma mass spectrometry, and mercury intrusion porosimetry revealed severe degradation of Pt nanoparticles (NPs), support structures, and the catalyst layer. Two degradation stages for NPs were proposed: Ostwald ripening dominated the initial 60,000 cycles, followed by combined Ostwald ripening and particle migration. Measurements with ion chromatography, high-frequency resistance, and oxygen-diffusion resistance revealed degradation of membrane and ionomer, respectively.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"20 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570281","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Artificial manganese nanozyme for nonradical activation of periodate toward pH-universal water decontamination 人工锰纳米酶非自由基活化高碘酸盐在ph -通用水净化中的应用

IF 9.4

Chem Catalysis Pub Date : 2025-03-04 DOI: 10.1016/j.checat.2025.101299

Minjia Yan, Jiahao Sun, Yujing Chen, Xixian Liu, Bowen Xu, Jianrong Chen, Feng Chen, Qianwei Liang, Shaobin Wang, Xi-Lin Wu, Xiaoguang Duan

{"title":"Artificial manganese nanozyme for nonradical activation of periodate toward pH-universal water decontamination","authors":"Minjia Yan, Jiahao Sun, Yujing Chen, Xixian Liu, Bowen Xu, Jianrong Chen, Feng Chen, Qianwei Liang, Shaobin Wang, Xi-Lin Wu, Xiaoguang Duan","doi":"10.1016/j.checat.2025.101299","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101299","url":null,"abstract":"Single-atom nanozymes (SAzymes), designed to mimic the active centers of natural enzymes, are emerging as a versatile catalytic platform for heterogeneous catalysis. Herein, enzyme-mimicking single-atom manganese (EMSA-Mn) sites supported on graphitic carbon nitride (g-C3N4) were constructed, marking a pioneering application of EMSA-Mn-C3N4 for periodate (PI; IO4−)-based advanced oxidation processes (AOPs). The EMSA-Mn-C3N4/PI system demonstrated remarkable efficiency in eliminating organic micropollutants across a broad pH range (pH 3–11). The positively charged EMSA-Mn sites facilitated the adsorption of the negatively charged IO4−, forming the EMSA-Mn-PI∗ complex, subsequently triggering a direct electron-transfer process (ETP) for oxidation of the organic pollutants. Experimental and theoretical results revealed that the EMSA-Mn site possesses higher intrinsic activity than conventional SA-Mn sites anchored on g-C3N4, thereby achieving higher efficiency for PI activation via the ETP. This work provides an advanced design strategy to construct Mn SAzymes for environmental catalysis and deeper insights into the nonradical PI-AOP systems.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"29 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143538342","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Zeolite composite prepared by quasi-in situ interzeolite conversion approach 准原位分子筛间转化法制备沸石复合材料

IF 9.4

Chem Catalysis Pub Date : 2025-03-04 DOI: 10.1016/j.checat.2025.101298

Ruizhe Zhang, Bo Wang, Jiani Xu, Honghai Liu, Hongjuan Zhao, Jiujiang Wang, Shutao Xu, Shunsuke Asahina, Francesco Dalena, Camille Longue, Benoît Louis, Ludovic Pinard, Simona Moldovan, Zhengxing Qin, Xionghou Gao, Svetlana Mintova

{"title":"Zeolite composite prepared by quasi-in situ interzeolite conversion approach","authors":"Ruizhe Zhang, Bo Wang, Jiani Xu, Honghai Liu, Hongjuan Zhao, Jiujiang Wang, Shutao Xu, Shunsuke Asahina, Francesco Dalena, Camille Longue, Benoît Louis, Ludovic Pinard, Simona Moldovan, Zhengxing Qin, Xionghou Gao, Svetlana Mintova","doi":"10.1016/j.checat.2025.101298","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101298","url":null,"abstract":"The design of zeolites with optimized textural properties is a continuous goal. Here, we report a composite comprising mesoporous ultra-stable zeolite Y (USY) and nanosized Zeolite Socony Mobil-5 (ZSM-5) with enhanced acid site accessibility and pore connectivity through quasi-in situ interzeolite conversion in a solvent-free medium. The preparation of the composite begins with a spatial and elemental-biased dissolution of USY with impregnated tetrapropylammonium hydroxide (TPAOH). This results in a hierarchical zeolite with increased mesopore volume and improved pore connectivity. Simultaneously, the solute provides all the necessary nutrients for the growth of ZSM-5 zeolite. Due to the constrained mass transfer during the quasi-solid-state dissolution, the resulting ZSM-5 crystals are as small as 10 nm and intimately connected with the USY zeolite. The advantageous synergy between zeolites Y and ZSM-5 in the composite was demonstrated through the methanol-to-olefin reaction and the cracking of n-hexane.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"85 2 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143538341","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0