Nature Catalysis最新文献_第4页

Semiconductors in pores 孔隙中的半导体

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-07-24 DOI: 10.1038/s41929-025-01385-8

Zhuo Jiang, Xiaofan Shi, Hexiang Deng

引用次数: 0

A radical way to ethylene 乙烯的自由基生成方法

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-07-24 DOI: 10.1038/s41929-025-01382-x

Luka Ðorđević, Francesca Arcudi

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Biocompatible Lossen rearrangement 生物相容性Lossen重排

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-07-24 DOI: 10.1038/s41929-025-01391-w

Jan-Stefan Völler

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Biomimetic aldol reaction of glycinate 甘氨酸的仿生醛醇反应

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-07-24 DOI: 10.1038/s41929-025-01383-w

Luca Bernardi

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Cobalt hydride-mediated photocatalytic semihydrogenation of acetylene impurities for continuous-flow production of polymer-grade ethylene 钴氢化介导乙炔杂质光催化半加氢连续流生产聚合级乙烯

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-07-22 DOI: 10.1038/s41929-025-01380-z

Haojie Dai, Yuhan Wang, Kailin Wang, Hao Kang, Xiangyang Chen, Bei Ding, Xudan Chen, Ying Du, Lize Dong, Wen Zhong, Ning Sun, Pengyu Liu, Chunyang Yu, Jingyuan Ma, Fei Song, Yongfeng Hu, Shan Tang, Yannan Liu, Wenfeng Jiang, Yuanhai Su, Jun Li, Yongfeng Zhou

{"title":"Cobalt hydride-mediated photocatalytic semihydrogenation of acetylene impurities for continuous-flow production of polymer-grade ethylene","authors":"Haojie Dai, Yuhan Wang, Kailin Wang, Hao Kang, Xiangyang Chen, Bei Ding, Xudan Chen, Ying Du, Lize Dong, Wen Zhong, Ning Sun, Pengyu Liu, Chunyang Yu, Jingyuan Ma, Fei Song, Yongfeng Hu, Shan Tang, Yannan Liu, Wenfeng Jiang, Yuanhai Su, Jun Li, Yongfeng Zhou","doi":"10.1038/s41929-025-01380-z","DOIUrl":"10.1038/s41929-025-01380-z","url":null,"abstract":"The semihydrogenation of acetylene impurities in crude ethylene streams to produce polymer-grade ethylene is important for the polyethylene industry. Photocatalytic reduction offers a promising solution in terms of sustainability. However, the current state of photocatalytic acetylene semihydrogenation systems has shown limited activity. Here we report a metal-catalysed hydrogen atom transfer pathway to promote photocatalytic acetylene semihydrogenation via rapid formation of cobalt hydride species. Applying a N,N′-bis(salicylidene)ethylenediamine cobalt catalyst with an electron-donating ligand that energetically favours cobalt hydride formation in pure acetylene yields excellent acetylene-to-ethylene reduction performance with near-unity selectivity, a turnover number of 29,401 and a turnover frequency of 2.14 s−1. Most importantly, we engineered a continuous-flow photoreactor, by which crude ethylene containing 1.10 vol% acetylene can be steadily converted into polymer-grade ethylene continuously over 50 h. Despite the ease of fine-tuning their reactivity, high-performance homogeneous photocatalysts competent for acetylene semihydrogenation are scarce. Here the authors introduce an effective cobalt catalyst for the production of polymer-grade ethylene, which is amenable to scale-up in a continuous-flow photoreactor.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 7","pages":"645-656"},"PeriodicalIF":44.6,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678209","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Controlling hydrocarbon chain growth and degree of branching in CO2 electroreduction on fluorine-doped nickel catalysts 含氟镍催化剂对CO2电还原过程中烃链生长及支化程度的控制

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-07-17 DOI: 10.1038/s41929-025-01370-1

Yingqing Ou, Lu Liu, Ranga Rohit Seemakurthi, Futian You, Haibin Ma, Javier Pérez-Ramírez, Núria López, Boon Siang Yeo

{"title":"Controlling hydrocarbon chain growth and degree of branching in CO2 electroreduction on fluorine-doped nickel catalysts","authors":"Yingqing Ou, Lu Liu, Ranga Rohit Seemakurthi, Futian You, Haibin Ma, Javier Pérez-Ramírez, Núria López, Boon Siang Yeo","doi":"10.1038/s41929-025-01370-1","DOIUrl":"10.1038/s41929-025-01370-1","url":null,"abstract":"Nickel-based materials can facilitate the electrocatalytic CO2 reduction (CO2R) reaction to generate hydrocarbons up to C6. Here we show that fluorine doping alters the nature of the Ni active sites, which proves instrumental in tuning the selectivity of the CO2R. We interrogate the CO2R reaction mechanism using intermediate surrogates, including aldehydes, alkyl iodides and acetylene. Aldehydes are electroreduced to alcohols and deoxygenated intermediates. Among the latter, unsaturated hydrocarbon intermediates (RCH2−x*, where the asterisk represents surface-bound species and x = 1 or 2) reacting with *CO dictate chain propagation, modulated by competitive C–C coupling and C–H hydrogenation reactions. Compound branching in the hydrocarbons initiates from *CO coupling with two *CH2 species, and the branch-to-linear hydrocarbon ratio can be doubled using a pulsed potential strategy. An inverse H/D kinetic isotope effect promotes deuterated hydrocarbon formation with a Faradaic efficiency of 22.2%. This work reveals mechanisms and strategies for the conversion of CO2 into linear and branched hydrocarbons, thus advancing electrosynthetic fuel development. Ni-based CO2 reduction electrocatalysts have been reported to produce multicarbon products up to C6 but with limited selectivity. Here the reaction mechanism of the process is elucidated. Consequently, pulsed potential electrolysis and electrolyte deuteration are respectively employed to enhance the selectivity of branched hydrocarbons and increase the total hydrocarbon Faradaic efficiency to 22%.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 7","pages":"714-727"},"PeriodicalIF":44.6,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144645256","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Selective electrooxidation of 5-hydroxymethylfurfural at pilot scale by engineering a solid polymer electrolyte reactor 固体聚合物电解质反应器中试规模下5-羟甲基糠醛选择性电氧化研究

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-07-17 DOI: 10.1038/s41929-025-01374-x

Yue Ren, Wei Kong, Yang Li, Wang Zhan, Chunyu Zhang, Yuhang Miao, Bingxin Yao, Shengnan Li, Zhenhua Li, Xiang Liu, Sheng Zhan, Hua Zhou, Mingfei Shao, Haohong Duan

{"title":"Selective electrooxidation of 5-hydroxymethylfurfural at pilot scale by engineering a solid polymer electrolyte reactor","authors":"Yue Ren, Wei Kong, Yang Li, Wang Zhan, Chunyu Zhang, Yuhang Miao, Bingxin Yao, Shengnan Li, Zhenhua Li, Xiang Liu, Sheng Zhan, Hua Zhou, Mingfei Shao, Haohong Duan","doi":"10.1038/s41929-025-01374-x","DOIUrl":"10.1038/s41929-025-01374-x","url":null,"abstract":"Aqueous electrolysis offers a potential sustainable route for converting biomass derivatives to plastic monomers, such as 5-hydroxymethylfurfural oxidation to 2,5-furandicarboxylic acid (FDCA). However, selective electrosynthesis of high-concentration FDCA at kilowatt scale and ampere-level current density remains an unmet challenge, hindering commercialization. Here we show an engineered solid polymer electrolyte (SPE) reactor to steer Faradaic and non-Faradaic side reactions, achieving FDCA production at an industrially relevant current density (1.5 A cm−2) while maintaining high selectivity (97.0%), Faradaic efficiency (88.2%) and concentration (~1.24 M). The stability of the SPE reactor was demonstrated in continuous operation at 0.5 A cm−2 over 140 h. Moreover, a 4.3-kW electrochemical platform was constructed with a scale-out strategy, reaching a pilot-scale FDCA production rate (33 kg per day). This work shows the capability of reactor engineering to enable selective and large-scale production of sustainable chemicals via electrochemical processes. Aqueous electroconversion of biomass derivatives to polymer precursors has been demonstrated at the laboratory scale with low yield. Here a solid polymer electrolyte reactor is engineered to limit side reactions, yielding a high rate and and a high product concentration in a 4.3-kW pilot-scale platform.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 8","pages":"771-783"},"PeriodicalIF":44.6,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144645403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Author Correction: Exploring mesoscopic mass transport effects on electrocatalytic selectivity 作者更正：探索介观质量输运对电催化选择性的影响

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-07-17 DOI: 10.1038/s41929-025-01393-8

Hendrik H. Heenen, Hemanth S. Pillai, Karsten Reuter, Vanessa J. Bukas

引用次数: 0

Boron clusters as efficient shuttles for electrocatalytic deuterium labelling via radical H/D exchange 硼团簇作为通过自由基H/D交换的电催化氘标记的有效穿梭体

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-07-15 DOI: 10.1038/s41929-025-01379-6

Meng He, Xuefan Deng, Fengze Yao, Yachun Wang, Yuan Gao, Pengjie Wang, Qiongqiong Wan, Kaixiang Chen, Liwei Wang, Hong Yi, Haibo Zhang, Wu Li, Aiwen Lei

{"title":"Boron clusters as efficient shuttles for electrocatalytic deuterium labelling via radical H/D exchange","authors":"Meng He, Xuefan Deng, Fengze Yao, Yachun Wang, Yuan Gao, Pengjie Wang, Qiongqiong Wan, Kaixiang Chen, Liwei Wang, Hong Yi, Haibo Zhang, Wu Li, Aiwen Lei","doi":"10.1038/s41929-025-01379-6","DOIUrl":"10.1038/s41929-025-01379-6","url":null,"abstract":"Deuterium labelling has widespread applications in medicinal chemistry, chemical science and materials science. Hydrogen isotope exchange for deuterium labelling of C(sp3)–H bonds under mild conditions remains a key challenge in labelling reactions. Here we show an electrocatalytic strategy enabling rapid (<10 min) deuteration of natural products and pharmaceuticals. Using clusters containing boron, (TBA)2B10H10, as the electrocatalyst, anodically generated [B10H10]•− intermediates undergo hydrogen-atom transfer with C(sp3)–H/D bonds, forming stabilized [B10H10H/D]− species. Cathodic reduction then triggers selective H/D exchange with carbon radicals, regenerating the catalyst. The boron cluster modulates reactive H/D radicals via reversible electron transfer, balancing radical activity and stability to enable efficient labelling without harsh reagents. This method achieves broad substrate compatibility and high deuterium incorporation and is demonstrated using complex drug molecules. By integrating electrocatalysis with boron cluster-mediated hydrogen-atom transfer, we provide a general platform for C(sp3)–H deuteration, advancing isotope-labelling applications in synthetic and medicinal chemistry. Methods for deuterium labelling of C–H bonds under mild conditions are sought after. Now an electrocatalytic method for H/D exchange via a radical-mediated pathway is described, using a boron cluster as a radical shuttle during the coupling process of deuterium and carbon radicals.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 8","pages":"784-793"},"PeriodicalIF":44.6,"publicationDate":"2025-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144629903","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Radical S-adenosyl-l-methionine FeS cluster implicated as the sulfur donor during albomycin biosynthesis 自由基s -腺苷-l-蛋氨酸FeS簇在白霉素生物合成过程中作为硫供体

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-07-15 DOI: 10.1038/s41929-025-01367-w

Richiro Ushimaru, Ziyang Zheng, Jin Xiong, Takahiro Mori, Ikuro Abe, Yisong Guo, Hung-wen Liu

{"title":"Radical S-adenosyl-l-methionine FeS cluster implicated as the sulfur donor during albomycin biosynthesis","authors":"Richiro Ushimaru, Ziyang Zheng, Jin Xiong, Takahiro Mori, Ikuro Abe, Yisong Guo, Hung-wen Liu","doi":"10.1038/s41929-025-01367-w","DOIUrl":"10.1038/s41929-025-01367-w","url":null,"abstract":"Carbon–sulfur bond-forming reactions in natural product biosynthesis largely involve Lewis acid/base chemistry with relatively few examples catalysed by radical S-adenosyl-l-methionine (SAM) enzymes. The latter have been limited to radical-mediated sulfur insertion into carbon–hydrogen bonds with the sulfur atom originating from a sacrificial auxiliary iron–sulfur cluster. Here we show that the radical SAM enzyme AbmM encoded in the albomycin biosynthetic gene cluster catalyses a sulfur-for-oxygen swapping reaction, transforming the furanose ring of cytidine 5′-diphosphate to a thiofuranose moiety that is essential for the antibacterial activity of albomycin δ2. Thus, in addition to its canonical function of mediating the reductive cleavage of SAM, the radical SAM catalytic cluster of AbmM appears to play a role in providing the sulfur introduced during the AbmM-catalysed reaction. These discoveries not only establish the origin of the thiofuranose core in albomycin δ2 but, more importantly, also emphasize the functional diversity of radical SAM catalysis. The mechanism by which sulfur is incorporated into the furanose ring in albomycins—a group of natural nucleoside antibiotics—remains unclear. Now, this work explains how twitch radical S-adenosyl-l-methionine enzyme AbmM catalyses sulfur-for-oxygen replacement in the biosynthesis of albomycin δ2.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 8","pages":"760-770"},"PeriodicalIF":44.6,"publicationDate":"2025-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144629902","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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