Chem Catalysis最新文献

Will biohybrid or tandem CO2 electrolysis prevail?

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

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

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

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

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

Enantioselective [2π + 2σ] cycloaddition of bicyclobutanes with imines: An efficient approach to chiral 2-aza-bicyclo[2.1.1]hexanes

IF 9.4

Chem Catalysis Pub Date : 2025-03-04 DOI: 10.1016/j.checat.2025.101295

Xuan-Ge Zhang, Jun-Jia Chen, Zi-Yang Zhou, Jia-Xin Li, Qi-Lin Zhou

引用次数: 0

Late-stage functionalization of pharmaceuticals by C–C cross-coupling enabled by wingtip-flexible N-heterocyclic carbenes

IF 9.4

Chem Catalysis Pub Date : 2025-02-28 DOI: 10.1016/j.checat.2025.101297

Shiyi Yang, Tongliang Zhou, Xiang Yu, Albert Poater, Josep Duran, Maciej Spiegel, Luigi Cavallo, Steven P. Nolan, Michal Szostak

{"title":"Late-stage functionalization of pharmaceuticals by C–C cross-coupling enabled by wingtip-flexible N-heterocyclic carbenes","authors":"Shiyi Yang, Tongliang Zhou, Xiang Yu, Albert Poater, Josep Duran, Maciej Spiegel, Luigi Cavallo, Steven P. Nolan, Michal Szostak","doi":"10.1016/j.checat.2025.101297","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101297","url":null,"abstract":"The synthesis of complex molecules by palladium-catalyzed cross-coupling has been pivotal in all stages of drug discovery research. However, this approach has been generally restricted to classical aryl halide electrophiles, requiring the use of a limited pool of precursors. Herein, we report the first highly chemoselective approach to the cross-coupling of bench-stable C–O electrophiles in which abundant phenols can be systematically used as electrophilic cross-coupling partners. Using this approach, we have achieved late-stage functionalization of >20 pharmaceuticals covering various architectures and drug targets. Wingtip-flexible N-heterocyclic carbenes as ancillary ligands enable us to address the major challenges to this mode of catalysis, such as fast oxidative addition to prevent the hydrolysis of C–O electrophiles and facile reductive elimination to establish C–C bond formation in complex settings. The design of wingtip-flexible N-heterocyclic carbene ligands will enable the cross-coupling of a broad range of electrophiles for the development of important medicines.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"24 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518290","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

CO2-to-C2H5OH photoconversion by an amorphization-activated catalyst

IF 9.4

Chem Catalysis Pub Date : 2025-02-28 DOI: 10.1016/j.checat.2025.101293

Fei Xue, Chunyang Zhang, Maochang Liu, Feng Liu, Xueli Yan, Shangheng Liu, Huiping Peng, Zhiwei Hu, Chih-Wen Pao, Wei-Hsiang Huang, Ye Yang, Xiaoqing Huang, Yong Xu

{"title":"CO2-to-C2H5OH photoconversion by an amorphization-activated catalyst","authors":"Fei Xue, Chunyang Zhang, Maochang Liu, Feng Liu, Xueli Yan, Shangheng Liu, Huiping Peng, Zhiwei Hu, Chih-Wen Pao, Wei-Hsiang Huang, Ye Yang, Xiaoqing Huang, Yong Xu","doi":"10.1016/j.checat.2025.101293","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101293","url":null,"abstract":"CO2 photoconversion into value-added C2 products with high selectivity and efficiency is formidably challenging due to highly energetic and kinetic restriction of C–C coupling. Designing catalysts to overcome those barriers is therefore crucial. Here, for the first time, we demonstrate an amorphization strategy to boost photocatalytic CO2 ethanolization. By integrating amorphous Pd onto Cd0.9Zn0.1S nanorods (a-Pd/CZS), an activity of 412.1 μmol g−1 h−1 and a selectivity of 96.5% for CO2-to-C2H5OH photoconversion were achieved without a sacrificial agent with an apparent quantum efficiency (AQE) of 0.87% at 420 nm. The superior performance results from rapid migration of photogenerated electrons to amorphous Pd via interfacial Ohmic junction. In situ characterization and theoretical calculation further reveal that amorphous Pd can optimize CO2 adsorption/activation and reduce the C–C coupling energy barrier via intensified interaction and stabilization with a ∗OCCO intermediate, thereby maximizing conversion efficiency and selectivity. This work highlights an efficient photocatalyst for a CO2-to-C2 product and inspires high-performance photocatalyst design.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"54 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518291","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

Mechanistic kinetic Monte Carlo modeling of the synthesis of hyperbranched polyesters

IF 9.4

Chem Catalysis Pub Date : 2025-02-26 DOI: 10.1016/j.checat.2025.101296

Matthew W. Coile, V. Sai Phani Kumar, Changxia Shi, Eugene Y.-X. Chen, Linda J. Broadbelt, Alexander Shaw

{"title":"Mechanistic kinetic Monte Carlo modeling of the synthesis of hyperbranched polyesters","authors":"Matthew W. Coile, V. Sai Phani Kumar, Changxia Shi, Eugene Y.-X. Chen, Linda J. Broadbelt, Alexander Shaw","doi":"10.1016/j.checat.2025.101296","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101296","url":null,"abstract":"Most plastics recycled today are recycled mechanically, often referred to as downcycling due to the inevitable degradation of the polymer material. One alternative is to chemically recycle these materials back to a monomer, but this works most efficiently for intrinsically circular polymers (iCPs) that exhibit appropriate depolymerization thermodynamics and kinetics. In order to help design such iCP materials, modeling can provide insight into the effect of reaction conditions on their polymerization and depolymerization characteristics. Most iCPs reported are linear polymers, so architecturally complex hyperbranched polymers that exhibit complete chemical circularity are rare, and modeling on hyperbranched iCPs has not been reported. Here, we report a mechanistic model that incorporates chain-length-dependent transport phenomena and tracks the full polymer structure during the reversible polymerization of a hydroxyl-functionalized lactone leading to this hyperbranched polyester. This lays the groundwork for future modeling of this material’s depolymerization behavior and provides a framework that can be employed to study other iCPs.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"4 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495761","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

Syngas production from the air

IF 9.4

Chem Catalysis Pub Date : 2025-02-24 DOI: 10.1016/j.checat.2024.101254

Yongqiang Wang, Jining Guo, Longbing Qu, Paul Webley, Hui Ding, Gang Kevin Li

引用次数: 0