Chem Catalysis最新文献_第2页

Close-loop chemical recycling unlocked via waste polyolefins-ethylene co-metathesis 通过废弃聚烯烃与乙烯的共甲氧基化反应实现闭环化学循环利用

IF 9.4

Chem Catalysis Pub Date : 2024-11-21 DOI: 10.1016/j.checat.2024.101194

Pavel A. Kots

引用次数: 0

Deoxygenative alcohol–nucleophile coupling via carbocations 通过碳化作用实现脱氧醇-核亲和剂偶联

IF 9.4

Chem Catalysis Pub Date : 2024-11-18 DOI: 10.1016/j.checat.2024.101187

Léa Thai-Savard, Jason R. Zbieg, Jack A. Terrett

引用次数: 0

Visible light-driven excited-state copper-BINAP catalysis for accessing diverse chemical reactions 利用可见光驱动激发态铜-BINAP 催化技术实现多样化化学反应

IF 9.4

Chem Catalysis Pub Date : 2024-11-15 DOI: 10.1016/j.checat.2024.101184

Upasana Mukherjee, Jagrut A. Shah, Ming-Yu Ngai

引用次数: 0

Metal cation exchange with zeolitic acid sites modulates hydrocarbon pool propagation during CO2 hydrogenation 金属阳离子与沸石酸位点的交换调节二氧化碳加氢过程中碳氢化合物池的扩散

IF 9.4

Chem Catalysis Pub Date : 2024-11-13 DOI: 10.1016/j.checat.2024.101183

Fatima Mahnaz, Balaji C. Dharmalingam, Jasan Robey Mangalindan, Jenna Vito, Jithin John Varghese, Manish Shetty

{"title":"Metal cation exchange with zeolitic acid sites modulates hydrocarbon pool propagation during CO2 hydrogenation","authors":"Fatima Mahnaz, Balaji C. Dharmalingam, Jasan Robey Mangalindan, Jenna Vito, Jithin John Varghese, Manish Shetty","doi":"10.1016/j.checat.2024.101183","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101183","url":null,"abstract":"We demonstrate that the exchange of zeolitic Brønsted acid sites (BASs) with cations from metal oxides plays a pivotal role in the propagation of hydrocarbon pools (HCPs) during CO2 hydrogenation. We probed the likelihood of In2O3, ZnZrOx, and Cr2O3 migration and their cation exchange with BASs of a silicoaluminophosphate, SAPO-34, by integrating them at nanoscale proximity (∼1,400 nm). Analysis with NH3 temperature-programmed desorption and transmission Fourier transform infrared spectroscopy showed ion exchange of BASs with Inδ+ and Znδ+ but not for Crδ+. We measured the C3/C2 hydrocarbon ratio (indicating relative propagation of olefin to aromatic cycles) and paraffin-to-olefin ratio, which revealed that Inδ+ species inhibited HCPs inside the channels of SAPO-34, while Znδ+ species enhanced hydrogen transfer and secondary hydrogenation. Combining reactivity data with occluded hydrocarbon analysis and 13C solid-state nuclear magnetic resonance spectroscopy, we show that ion-exchanged species affect HCP propagation. Overall, our work provides insights for the rational integration of bifunctional catalysts.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"3 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601710","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

Symmetry-breaking CoN3S1 centers enable inert chloride ion adsorption for facilitating self-driven overall seawater splitting 打破对称的 CoN3S1 中心可实现惰性氯离子吸附，从而促进自驱动的整体海水分离

IF 9.4

Chem Catalysis Pub Date : 2024-11-12 DOI: 10.1016/j.checat.2024.101169

Canhui Zhang, Xu Liu, Cheng Zhen, Hanxu Yao, Liangliang Xu, Haibing Ye, Yue Wang, Xingkun Wang, M. Danny Gu, Minghua Huang, Heqing Jiang

{"title":"Symmetry-breaking CoN3S1 centers enable inert chloride ion adsorption for facilitating self-driven overall seawater splitting","authors":"Canhui Zhang, Xu Liu, Cheng Zhen, Hanxu Yao, Liangliang Xu, Haibing Ye, Yue Wang, Xingkun Wang, M. Danny Gu, Minghua Huang, Heqing Jiang","doi":"10.1016/j.checat.2024.101169","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101169","url":null,"abstract":"A self-driven seawater splitting system could efficiently produce hydrogen from abundant seawater. However, high Cl− concentrations in seawater lead to catalyst corrosion and deactivation, impairing performance in the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). Here, we adopted single-atom Co-N-C-based catalysts, in which the electronic structure around the central Co site can be controlled and adjusted at an atomic level. Experimentally, the target N and S co-doped hollow carbon sphere (Co-N/S-HCS) catalyst, featuring asymmetric Co-N3S1 sites, shows excellent ORR/OER/HER performance. By employing density functional theory and molecular dynamics simulations of real-time simulations, we reveal that the S doped in the asymmetric Co-N3S1 model leads to a customized electronic structure around the central Co site, enabling weakened adsorption of the corrosive Cl− and excellent ORR/OER/HER activities. Moreover, the seawater-based Zn-air batteries (S-ZABs) assembled by the Co-N/S-HCS deliver a cycling performance exceeding 650 h, and the overall seawater splitting system can run continuously for 1,100 h.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"71 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599720","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

Illuminating selectivity descriptors for the methanol-to-propylene process over Ca-modified and unmodified zeolite ZSM-5 甲醇制丙烯工艺在钙改性和未改性沸石 ZSM-5 上的光照选择性描述符

IF 9.4

Chem Catalysis Pub Date : 2024-11-12 DOI: 10.1016/j.checat.2024.101168

Abhay Dokania, Xuan Gong, Edy Abou-Hamad, Alla Dikhtiarenko, Tuiana Shoinkhorova, Yiru Ye, Javier Patarroyo, Nimer Wehbe, Abhishek Dutta Chowdhury, Jorge Gascon

{"title":"Illuminating selectivity descriptors for the methanol-to-propylene process over Ca-modified and unmodified zeolite ZSM-5","authors":"Abhay Dokania, Xuan Gong, Edy Abou-Hamad, Alla Dikhtiarenko, Tuiana Shoinkhorova, Yiru Ye, Javier Patarroyo, Nimer Wehbe, Abhishek Dutta Chowdhury, Jorge Gascon","doi":"10.1016/j.checat.2024.101168","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101168","url":null,"abstract":"There is a growing demand for propylene calls for effective carbon reduction methods. The methanol-to-propylene (MTP) process stands out as a promising solution for meeting global propylene demand sustainably. In this study, we identify the mechanistic factors responsible for enhanced reactivity, superior propylene selectivity, and durable catalyst lifespan in the MTP process catalyzed by both unmodified siliceous and Ca-modified ZSM-5 zeolites. By employing advanced characterization techniques like in situ UV-visible and solid-state NMR spectroscopy, along with well-designed control experiments, we highlight the importance of the alkene cycle within the zigzag channel of zeolite ZSM-5 for superior propylene selectivity. Furthermore, our work identifies oxymethylene species as a key intermediate that enhances the lifetime of the alkene cycle and governs MTP catalysis. We also explore the synergistic interaction between Lewis-Brønsted acids and their impact on hydrocarbon pool species to deepen our understanding of zeolite catalysis.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"19 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599687","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

Shifting hydrogenation pathway via electronic activation for efficient nitrate electroreduction to ammonia in sewages 通过电子活化改变氢化途径，在污水中将硝酸盐高效电还原为氨气

IF 9.4

Chem Catalysis Pub Date : 2024-11-12 DOI: 10.1016/j.checat.2024.101182

Wenye Zhong, Xuepeng Xiang, Peiyan Chen, Jiayu Su, Zhiheng Gong, Xueming Liu, Shijun Zhao, Nian Zhang, Chunhua Feng, Zhibin Zhang, Yan Chen, Zhang Lin

{"title":"Shifting hydrogenation pathway via electronic activation for efficient nitrate electroreduction to ammonia in sewages","authors":"Wenye Zhong, Xuepeng Xiang, Peiyan Chen, Jiayu Su, Zhiheng Gong, Xueming Liu, Shijun Zhao, Nian Zhang, Chunhua Feng, Zhibin Zhang, Yan Chen, Zhang Lin","doi":"10.1016/j.checat.2024.101182","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101182","url":null,"abstract":"Electrochemical hydrogenation reactions have attracted worldwide attention as a sustainable alternative to thermo-catalytic hydrogenations. Nevertheless, the Faradaic efficiency, in many cases, is limited by the competing side reaction of hydrogen evolution. In this work, we demonstrate that the hydrogenation pathway can be effectively modulated by electronic activation near the interface. In a heterostructure consisting of a Cu foam matrix and Co3O4 decoration layer (Co@Cu), the surface Co is effectively activated by electrons transferring from underneath Cu, leading to strongly promoted reactant adsorption and weakened Co-H bonding. Consequently, the hydrogenation pathway on the Co site shifts from H-H coupling to nitrate reduction, resulting in an outstanding nitrate reduction reaction (NO3−RR) Faradaic efficiency of 97.67%. A hybrid reactor combining electroreduction and membrane separation is further constructed to realize an NH3 recovery rate as high as 857.1 g-N m−2 d−1 from actual sewage. The results can be generalized for other electrochemical hydrogenation reactions for energy and environment applications.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"33 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599718","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

Intermittent CO2 electrolysis needs its time in the sun 间歇式二氧化碳电解需要阳光下的时间

IF 9.4

Chem Catalysis Pub Date : 2024-11-06 DOI: 10.1016/j.checat.2024.101166

Izak Minnie, Hyunjik K. Kim, John Flake, Dongxia Liu

引用次数: 0

Discovery of the threshold potential that triggers photochemical water oxidation with Ru(II) photosensitizers and MOx catalysts 利用 Ru(II) 光敏剂和 MOx 催化剂发现引发光化学水氧化的阈值电位

IF 9.4

Chem Catalysis Pub Date : 2024-11-04 DOI: 10.1016/j.checat.2024.101167

Megumi Okazaki, Yasuomi Yamazaki, Daling Lu, Shunsuke Nozawa, Osamu Ishitani, Kazuhiko Maeda

{"title":"Discovery of the threshold potential that triggers photochemical water oxidation with Ru(II) photosensitizers and MOx catalysts","authors":"Megumi Okazaki, Yasuomi Yamazaki, Daling Lu, Shunsuke Nozawa, Osamu Ishitani, Kazuhiko Maeda","doi":"10.1016/j.checat.2024.101167","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101167","url":null,"abstract":"Photochemical water oxidation in the presence of a Ru(II) photosensitizer to form O2 is one of the most studied reactions in (photo)catalysis for both homogeneous and heterogeneous systems. In the present work, several Ru(II)-tris-diimine-type complexes with different ligands were used under a wide pH range (3.7–9.4) and over different transition-metal oxide (MOx) catalysts to reveal the factors that govern the O2 evolution activity. Most importantly, the results clarified that a certain “threshold” potential determines whether water oxidation can proceed and that this potential is related to the energy barrier for electron transfer from the MOx catalyst to the Ru(II) photosensitizer. The results of this work highlight that the potential of the electrons involved in the water oxidation on MOx catalysts can be estimated through the simple application of a photochemical reaction, which will be a useful measure for assessing the water oxidation activity of suspended nanoparticle catalysts.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"62 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574614","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

Singly and doubly oxidized carbenes and their applications in catalysis 单氧化和双氧化碳烯及其在催化中的应用

IF 9.4

Chem Catalysis Pub Date : 2024-11-04 DOI: 10.1016/j.checat.2024.101159

Alexis K. Day, Mehdi Abdellaoui, Michèle Soleilhavoup, Guy Bertrand

引用次数: 0