Chem Catalysis最新文献_第4页

Photothermal transformation of ethane to ethylene oxide via consecutive dehydrogenation and epoxidation reactions 乙烷通过连续脱氢和环氧化反应光热转化为环氧乙烷

IF 9.4

Chem Catalysis Pub Date : 2025-06-04 DOI: 10.1016/j.checat.2025.101417

Lingzhen Zeng, Zeyan Cen, Xingwu Liu, Tiancheng Pu, Haoyi Tang, Maolin Wang, Kaiyu Zhu, Jiarui Li, Meng Wang, Ding Ma

{"title":"Photothermal transformation of ethane to ethylene oxide via consecutive dehydrogenation and epoxidation reactions","authors":"Lingzhen Zeng, Zeyan Cen, Xingwu Liu, Tiancheng Pu, Haoyi Tang, Maolin Wang, Kaiyu Zhu, Jiarui Li, Meng Wang, Ding Ma","doi":"10.1016/j.checat.2025.101417","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101417","url":null,"abstract":"Integrating green and sustainable energy solutions is critical for improving both economic viability and environmental sustainability in chemical transformation. This work demonstrates a tandem process for ethylene oxide production from ethane, coupling ethane dehydrogenation and ethylene epoxidation, using solar irradiation as the sole energy source. The process employs photothermal tandem reactors, with oxygen introduced into the second reactor after dehydrogenation. Reaction temperatures were precisely controlled by modulating light intensity (∼940 K for dehydrogenation and ∼540 K for epoxidation). A NiLa/BN catalyst exhibited exceptional activity (152 mmol g−1 h−1) and stability for photocatalytic ethane dehydrogenation under sunlight, while the Ag-based catalyst facilitated the epoxidation reaction. The integrated system achieved 60% ethane conversion and 14% ethylene oxide yield. This study highlights the feasibility of using sunlight as a sustainable energy source for industrial chemical transformations, offering a potential way to reduce dependence on fossil fuels and decrease carbon emissions.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"15 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211603","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

Surface electron-donor-boosting single-atom nickel sites for CO2 electroreduction in pure water 纯水中CO2电还原的表面电子供体增强单原子镍位

IF 9.4

Chem Catalysis Pub Date : 2025-06-03 DOI: 10.1016/j.checat.2025.101416

Xiaoxiong Huang, Linping Qian, Yujin Ji, Wenzhe Niu, Yuncheng Hu, Liangyao Xue, Jingjing Li, Shuanglong Huang, Jiaqi Zhang, Youyong Li, Bo Zhang

{"title":"Surface electron-donor-boosting single-atom nickel sites for CO2 electroreduction in pure water","authors":"Xiaoxiong Huang, Linping Qian, Yujin Ji, Wenzhe Niu, Yuncheng Hu, Liangyao Xue, Jingjing Li, Shuanglong Huang, Jiaqi Zhang, Youyong Li, Bo Zhang","doi":"10.1016/j.checat.2025.101416","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101416","url":null,"abstract":"The electrocatalytic carbon dioxide reduction reaction (CO2RR) in pure water is one of the most promising strategies for avoiding crystallization in conventional electrolytes. Here, we sought to modify the catalyst of dispersed single-atom nickel (Ni) sites on an ultrathin nitrogen-doped carbon nanosheet (Ni–N–C) by using amino groups (Ni–N–C–NH2). The obtained Ni–N–C–NH2 catalysts exhibited a peak turnover frequency of 11.1 s−1 with >90% CO selectivity and ultrastable durability of 100 h of continuous operation and achieved two to three times greater current density than Ni–N–C. Operando spectroscopic evidence combined with theory studies suggested that the improved CO selectivity originates from the synergistic effect of the amino groups and Ni–N–C. The introduced amino groups with the surface property of the electron donor upshift the d-band center of Ni and favor CO2 capture and proton-coupled electron transfer, ultimately enabling highly efficient operation of the CO2RR on Ni–N–C catalysts.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"54 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144202364","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

Upcycling CO2 into succinic acid (C4H6O4) by cascading CO2 electroreduction with electrocarboxylation 通过级联CO2电还原和电羧化将CO2升级为琥珀酸（C4H6O4）

IF 9.4

Chem Catalysis Pub Date : 2025-06-03 DOI: 10.1016/j.checat.2025.101415

Junjun Mao, Dan Wang, Chenchen Zhang, Yuanming Xie, Qingqing Song, Bo Zhang, Yang Lou, Chengsi Pan, Jiawei Zhang, Ying Zhang, Yongfa Zhu

{"title":"Upcycling CO2 into succinic acid (C4H6O4) by cascading CO2 electroreduction with electrocarboxylation","authors":"Junjun Mao, Dan Wang, Chenchen Zhang, Yuanming Xie, Qingqing Song, Bo Zhang, Yang Lou, Chengsi Pan, Jiawei Zhang, Ying Zhang, Yongfa Zhu","doi":"10.1016/j.checat.2025.101415","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101415","url":null,"abstract":"Extending carbon dioxide (CO2) electrocatalysis to afford energy-rich carbohydrates with long carbon chains is significant but still suffers from unsatisfactory selectivity for products with more than three carbon atoms. Here, using CO2 as the only carbon feedstock, we present a cascade electrolysis strategy for succinic acid (SA; C4H6O4) synthesis by coupling CO2 electroreduction with electrocarboxylation of in situ-generated ethylene (C2H4). An overall CO2-to-C4H6O4 conversion was achieved. Our findings illustrate that adsorption of in situ-generated C2H4 and the rate-determining step (∗C2H4 to ∗C2H4COO) occur more easily over FeNi foam. Notably, compared with typical CO2 reduction products, converting gaseous CO2 into SA lowers separation costs, enhancing economic viability. Our strategy also significantly reduces carbon emissions (−0.174 kg CO2 per kg SA), compared with conventional strategies (1.94 for petrochemical and 0.88 for bio-based SA). This system accelerates CO2 conversion into long-chain carbohydrates, facilitating reintegration of this industrial waste gas into the global economy.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"15 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144202363","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

Which and how oxygen-containing functional groups on Ni@Graphene boost efficient hydrogenation via hydrogen spillover Ni@Graphene上哪些含氧官能团通过氢溢出促进高效氢化

IF 9.4

Chem Catalysis Pub Date : 2025-05-28 DOI: 10.1016/j.checat.2025.101412

Yuansen Zhang, Chenyang Shen, Xinran Xie, Kaidi Liu, Qiuyue Wang, Yongting Li, Yongzheng Wang, Qiaolun Liu, Weiping Ding, Xuefeng Guo

{"title":"Which and how oxygen-containing functional groups on Ni@Graphene boost efficient hydrogenation via hydrogen spillover","authors":"Yuansen Zhang, Chenyang Shen, Xinran Xie, Kaidi Liu, Qiuyue Wang, Yongting Li, Yongzheng Wang, Qiaolun Liu, Weiping Ding, Xuefeng Guo","doi":"10.1016/j.checat.2025.101412","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101412","url":null,"abstract":"Unveiling the impact mechanism of oxygen-containing functional groups (OFGs) on the hydrogen spillover and hydrogenation process of metal-carbon composite catalysts is crucial yet challenging. Multiple hydrogenation sites on traditional supported catalysts complicate clarifying the role of OFGs. Herein, we fabricate a series of Ni@Graphene catalysts with different OFG contents and types to study the influence of OFGs on the hydrogen spillover and the hydrogenation activity. The investigation indicates that, among all OFGs, phenol and carboxyl groups play a leading role by reducing the energy barrier for hydrogen atom migration and show a significant linear correlation with hydrogen spillover capacity, the latter further linearly boosts the hydrogenation activity (increased by 193%–239%), which can serve as effective descriptor of the activities of Ni@Graphene. This study not only unveils which and how OFGs enhance hydrogen spillover and catalytic hydrogenation activity but also provides insights and new strategies for designing high-performance hydrogenation catalysts.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"82 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144154053","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

Cp∗Rh(III)-catalyzed enantioselective C(sp3)–H amidation of azine-linked cyclobutanes Cp * Rh（III）催化的对映选择性C(sp3) -H酰胺化

IF 9.4

Chem Catalysis Pub Date : 2025-05-28 DOI: 10.1016/j.checat.2025.101413

Xing Xu, Heyao Shi, Dong-Hang Tan, Phillip Biallas, Alistair J.M. Farley, Christophe Genicot, Ken Yamazaki, Darren J. Dixon

引用次数: 0

Blue light-induced 1,4-aminoalkylation of 1,3-dienes enabled by N-heterocyclic carbene-Ir(III) catalysis 用n -杂环碳- ir （III）催化蓝光诱导1,3-二烯的1,4-氨基烷基化

IF 9.4

Chem Catalysis Pub Date : 2025-05-28 DOI: 10.1016/j.checat.2025.101414

Qi-Long Chen, Le Mao, Yi-Fan Pan, Bin Wang, Ka Lu, Zhiwei Jiao, Fu-Min Zhang, Xiao-Ming Zhang, Yong-Qiang Tu

{"title":"Blue light-induced 1,4-aminoalkylation of 1,3-dienes enabled by N-heterocyclic carbene-Ir(III) catalysis","authors":"Qi-Long Chen, Le Mao, Yi-Fan Pan, Bin Wang, Ka Lu, Zhiwei Jiao, Fu-Min Zhang, Xiao-Ming Zhang, Yong-Qiang Tu","doi":"10.1016/j.checat.2025.101414","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101414","url":null,"abstract":"The precise alkylamination difunctionalization of 1,3-dienes represents an efficient method for synthesizing valuable allylic amines. Here, we present an efficient visible light-induced uncommon 1,4-aminoalkylation of 1-substituted 1,3-diene derivatives by developing novel N-heterocyclic carbene (NHC)-Ir(III) complex as the photocatalyst. Various allylic amines, which are difficult to obtain through other transformations so far reported, can be obtained with good to excellent yields and regio-, diastereoselectivities by using N-hydroxyphthalimide esters as both alkyl and amino precursors. The broad substrate scope and distinct 1,4-regioselectivity offer a unique supplementary approach to the established transition metal-catalyzed 3,4-aminoalkylation of 1-substituted 1,3-dienes; mechanistic studies indicate that blue light-induced allylic radical/cation crossover mediated by the photocatalyst and the π-π stacking between the phthalimidyl unit and the aryl substrates also play a crucial role in the regioselective transformation, demonstrating the superiority of this NHC-Ir(III) photocatalytic system in current cascade alkylamination transformation.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"18 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144154054","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

Engineering PHL7 for improved poly(ethylene terephthalate) depolymerization via rational design and directed evolution 工程PHL7通过合理设计和定向进化改进聚对苯二甲酸乙酯解聚

IF 9.4

Chem Catalysis Pub Date : 2025-05-26 DOI: 10.1016/j.checat.2025.101399

Thomas M. Groseclose, Erin Kober, Matilda Clark, Benjamin Moore, Ramesh K. Jha, Zoe K. Taylor, Lexy A. Lujan, Gregg T. Beckham, Andrew R. Pickford, Taraka Dale, Hau B. Nguyen

{"title":"Engineering PHL7 for improved poly(ethylene terephthalate) depolymerization via rational design and directed evolution","authors":"Thomas M. Groseclose, Erin Kober, Matilda Clark, Benjamin Moore, Ramesh K. Jha, Zoe K. Taylor, Lexy A. Lujan, Gregg T. Beckham, Andrew R. Pickford, Taraka Dale, Hau B. Nguyen","doi":"10.1016/j.checat.2025.101399","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101399","url":null,"abstract":"Enzymatic depolymerization of poly(ethylene terephthalate) (PET) has emerged as a promising approach for polyester recycling, and, to date, many natural and engineered PET hydrolase enzymes have been reported. For industrial use, PET hydrolases must achieve high depolymerization extent and exhibit excellent thermostability. Here, we engineered a natural PET hydrolase, Polyester Hydrolase Leipzig #7 (PHL7), through rational design and directed evolution using a high-throughput screening platform. Four new enzymes were engineered with enhanced properties compared with the parent enzyme, wild-type PHL7 (PHL7-WT), and other benchmark PET hydrolases, under the tested conditions. In bioreactors, the exemplary engineered enzyme, PHL7-Jemez, exhibited improved ability to depolymerize amorphous PET film compared with PHL7-WT at 2.9% and 20% substrate loadings, with 37% and 270% higher hydrolysis, respectively, after 48 h. This study develops several state-of-the-art PET hydrolases and demonstrates a directed evolution platform to engineer high-performance enzymes, which can accelerate enzyme discovery toward improved biocatalytic recycling.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"34 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144137208","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

Historical and recent advances in enantioselective NHC-catalyzed radical reactions 对映选择性nhc催化自由基反应的历史和最新进展

IF 9.4

Chem Catalysis Pub Date : 2025-05-26 DOI: 10.1016/j.checat.2025.101398

Jia Song, Shi-Chao Ren, Yingguo Liu, Yonggui Robin Chi

引用次数: 0

Mechanistic rules for de novo design of enzymes 酶从头设计的机制规则

IF 9.4

Chem Catalysis Pub Date : 2025-05-23 DOI: 10.1016/j.checat.2025.101394

Michalis Chatzittofi, Jaime Agudo-Canalejo, Ramin Golestanian

引用次数: 0

Operando fluorescence spectroscopy for evaluating the activity of fatty acid hydrogenation catalysts 荧光光谱法评价脂肪酸加氢催化剂的活性