Nature Catalysis最新文献_第7页

Repurposing organic pollutants 有机污染物的再利用

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-26 DOI: 10.1038/s41929-024-01203-7

Francesco Zamberlan

引用次数: 0

Frustration-driven efficiency 挫折驱动效率

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-26 DOI: 10.1038/s41929-024-01202-8

Chenyu Wang

引用次数: 0

Identifying the activity of nanocatalyst sites 确定纳米催化剂位点的活性

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-26 DOI: 10.1038/s41929-024-01188-3

Woong Hee Lee

引用次数: 0

CO2-to-methanol electroconversion on a molecular cobalt catalyst facilitated by acidic cations 酸性阳离子促进分子钴催化剂上的二氧化碳-甲醇电转化

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-22 DOI: 10.1038/s41929-024-01197-2

Sunmoon Yu, Hiroki Yamauchi, Shuo Wang, Abhishek Aggarwal, Junghwa Kim, Kiarash Gordiz, Botao Huang, Hongbin Xu, Daniel J. Zheng, Xiao Wang, Haldrian Iriawan, Davide Menga, Yang Shao-Horn

{"title":"CO2-to-methanol electroconversion on a molecular cobalt catalyst facilitated by acidic cations","authors":"Sunmoon Yu, Hiroki Yamauchi, Shuo Wang, Abhishek Aggarwal, Junghwa Kim, Kiarash Gordiz, Botao Huang, Hongbin Xu, Daniel J. Zheng, Xiao Wang, Haldrian Iriawan, Davide Menga, Yang Shao-Horn","doi":"10.1038/s41929-024-01197-2","DOIUrl":"10.1038/s41929-024-01197-2","url":null,"abstract":"The crucial role of electrolyte cations in CO2 electroreduction has received intensive attention. One prevailing theory is that through electrostatic interactions or direct coordination, larger cations such as Cs+ can better stabilize the key intermediate species for CO and multicarbon (C2+) product generation, for example, on silver and copper, respectively. Here we show that smaller, more acidic alkali metal cations greatly enhance CO2-to-methanol conversion kinetics (Li+ > Na+ > K+ > Cs+) on an immobilized molecular cobalt catalyst, unlike the trend observed for CO and C2+. Through electrokinetic analyses and kinetic isotope effect studies along with computational investigations, we show that the hydration shell of a cation serves as a proton donor in the rate-determining protonation step of adsorbed CHO where acidic cations promote the proton-coupled electron transfer. This study reveals the promotional effect of cation solvation environment on CO2 electroreduction beyond the widely acknowledged stabilizing effect of cations. The non-innocence of electrolyte cations in the activity of CO2 reduction has been widely acknowledged, although these complex effects are not fully understood. Here, opposite to the trend observed with Cu and Ag surfaces, smaller alkali cations greatly enhance CO2-to-methanol conversion on a cobalt molecular electrocatalyst.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 9","pages":"1000-1009"},"PeriodicalIF":42.8,"publicationDate":"2024-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141737072","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

Long-range enhancements of micropollutant adsorption on metal-promoted photocatalysts 金属促进的光催化剂对微污染物的长程吸附增强作用

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-19 DOI: 10.1038/s41929-024-01199-0

Ming Zhao, Wenjie Li, Muwen Yang, Zhiheng Zhao, Rong Ye, Xianwen Mao, Paul Padgett, Peng Chen

{"title":"Long-range enhancements of micropollutant adsorption on metal-promoted photocatalysts","authors":"Ming Zhao, Wenjie Li, Muwen Yang, Zhiheng Zhao, Rong Ye, Xianwen Mao, Paul Padgett, Peng Chen","doi":"10.1038/s41929-024-01199-0","DOIUrl":"10.1038/s41929-024-01199-0","url":null,"abstract":"Photocatalysis can effectively degrade emerging (micro)pollutants in wastewater and achieve advanced water treatment objectives, wherein the low solar energy conversion efficiency remains a challenge. One key determinant is the effective adsorption of micropollutants, which is challenging to define, especially for photocatalysts with surface heterogeneity over different length scales and under (non-)reactive conditions. Here we report a generalizable imaging technique adCOMPEITS (adsorption-based competition-enabled imaging technique with super-resolution) and quantify the adsorption behaviours of non-fluorescent micropollutants on heterostructured Au/TiO2 photocatalysts at nanometre resolution under both non-catalytic and photo(electro)catalytic conditions. We discover a long-range enhancement of micropollutant adsorption on TiO2, which reaches micrometre-length scale and stems from the long-range surface band bending of TiO2 upon contacting metal co-catalyst. We further engineer the band bending to effectively modulate the long-range effects on molecular adsorption. The imaging technique and the scientific discoveries here should open avenues towards understanding and engineering metal-promoted photocatalysts for many applications. Methods for studying the adsorption behaviour of molecules onto surfaces under reactive and non-reactive conditions are needed to improve photocatalysts for water treatment. Here the authors develop an imaging technique, adCOMPEITS, to quantify the adsorption of micropollutants on Au/TiO2 and identify a long-range enhancement effect.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 8","pages":"912-920"},"PeriodicalIF":42.8,"publicationDate":"2024-07-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141725931","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

Electrocatalytic cyclic deracemization enabled by a chemically modified electrode 通过化学修饰电极实现电催化循环脱盐

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-11 DOI: 10.1038/s41929-024-01189-2

Cheng-Jie Zhu, Xiuying Yang, Jianchun Wang

{"title":"Electrocatalytic cyclic deracemization enabled by a chemically modified electrode","authors":"Cheng-Jie Zhu, Xiuying Yang, Jianchun Wang","doi":"10.1038/s41929-024-01189-2","DOIUrl":"10.1038/s41929-024-01189-2","url":null,"abstract":"Redox chemistry, which is frequently encountered in the formation of new bonds and stereocentres, relies on the compatibility of redox potentials. Despite recent advances, achieving a general electrocatalytic cyclic deracemization process without stoichiometric redox reagents remains a formidable challenge. Here we show that electrocatalytic cyclic deracemization of secondary alcohols can be accomplished through sequential iridium-catalysed enantioselective anodic dehydrogenation and rhodium-catalysed cathodic hydrogenation, utilizing metal hydride catalysis. A considerable hurdle arises as stronger hydride donors necessitate parent metal complexes to possess low reduction potentials, resulting in inherent redox potential incompatibility. Nonetheless, we overcame this incompatibility by leveraging a recyclable rhodium-catalyst-modified electrode as the cathode—an accomplishment that homogeneous rhodium catalysis could not achieve. Our approach enables chemoselective stereochemical editing of bioactive compounds with remarkable functional group tolerance. Surface characterization and mechanistic studies showcased the unique advantages conferred by the chemically modified electrode. Methods for electrocatalytic deracemization remained elusive. Now, electrocatalytic cyclic deracemization of alcohols is reported, involving sequential anodic dehydrogenation and cathodic hydrogenation using two distinct metal hydride catalysts and a chemically modified electrode to avoid redox incompatibility.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 8","pages":"878-888"},"PeriodicalIF":42.8,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141584432","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

Remote site-selective arene C–H functionalization enabled by N-heterocyclic carbene organocatalysis 通过 N-杂环碳烯有机催化实现远程位点选择性炔烃 C-H 功能化

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-11 DOI: 10.1038/s41929-024-01194-5

Qing-Zhu Li, Wen-Lin Zou, Zhao-Yuan Yu, Xin-Xin Kou, Yan-Qing Liu, Xiang Zhang, Yu He, Jun-Long Li

{"title":"Remote site-selective arene C–H functionalization enabled by N-heterocyclic carbene organocatalysis","authors":"Qing-Zhu Li, Wen-Lin Zou, Zhao-Yuan Yu, Xin-Xin Kou, Yan-Qing Liu, Xiang Zhang, Yu He, Jun-Long Li","doi":"10.1038/s41929-024-01194-5","DOIUrl":"10.1038/s41929-024-01194-5","url":null,"abstract":"Catalytic site-selective functionalization of distal C–H bonds represents a formidable challenge in organic synthesis. Particularly, the precise functionalization of distal aromatic C(sp2)–H bonds remains largely unexplored. Here we present a highly para-selective acylation strategy to target ultraremote aryl C(sp2)–H bonds, eight chemical bonds away from an activated functionality, through radical N-heterocyclic carbene organocatalysis. This method is developed on the basis of a unique single-electron pathway involving the site-selective activation of aryl C–H bonds by a nitrogen-centred radical generated in situ. Importantly, this organocatalytic approach shows potential for the functionalization of drugs, amino acids and peptides, thus highlighting its importance for medicinal chemistry. Our investigation encompassed meticulous mechanistic studies, including control experiments and density functional theory calculations, to unravel the intricacies behind the observed site selectivity and shed light on the mechanism of radical N-heterocyclic carbene organocatalysis. The precise functionalization of distant aromatic C(sp2)–H bonds remains largely unexplored. Here the authors report a para-selective acylation strategy to target remote aryl C(sp2)–H bonds away from an activated functionality through radical N-heterocyclic carbene organocatalysis.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 8","pages":"900-911"},"PeriodicalIF":42.8,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141584433","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

Key role of paracrystalline motifs on iridium oxide surfaces for acidic water oxidation 氧化铱表面副晶图案在酸性水氧化中的关键作用

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-10 DOI: 10.1038/s41929-024-01187-4

Bingzhang Lu, Carolin Wahl, Roberto dos Reis, Jane Edgington, Xiao Kun Lu, Ruihan Li, Matthew E. Sweers, Brianna Ruggiero, G. T. Kasun Kalhara Gunasooriya, Vinayak Dravid, Linsey C. Seitz

{"title":"Key role of paracrystalline motifs on iridium oxide surfaces for acidic water oxidation","authors":"Bingzhang Lu, Carolin Wahl, Roberto dos Reis, Jane Edgington, Xiao Kun Lu, Ruihan Li, Matthew E. Sweers, Brianna Ruggiero, G. T. Kasun Kalhara Gunasooriya, Vinayak Dravid, Linsey C. Seitz","doi":"10.1038/s41929-024-01187-4","DOIUrl":"10.1038/s41929-024-01187-4","url":null,"abstract":"Water electrolysis using proton exchange membrane technology offers an ideal process for green hydrogen production, but widespread deployment is inhibited by insufficient catalyst activity, stability and affordability. Iridium-based oxides provide the best overall performance for acidic water oxidation, the limiting reaction for this process, but further improvements are impeded by poor understanding of the restructured active catalyst surface that forms under reaction conditions. Here we present a combination of X-ray and electron scattering data that reveals direct evidence for three paracrystalline structural motifs at the restructured surfaces of highly active catalysts (including rutile IrO2 and perovskite SrIrO3) that have previously been described as amorphous. These insights enable the design of a paracrystalline IrOx catalyst that is independent of the bulk crystalline support and maintains higher activity, longer stability and more effective use of iridium to promote the production of green hydrogen. Iridium-based oxides are the most active catalysts for acidic water oxidation, but a complete understanding of their surface reconstruction under operation remains elusive. Now three key paracrystalline structural motifs are identified on the seemingly amorphous reconstructed IrOx surface.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 8","pages":"868-877"},"PeriodicalIF":42.8,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141566319","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

Atomic-scale identification of active sites of oxygen reduction nanocatalysts 氧还原纳米催化剂活性位点的原子尺度鉴定

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-08 DOI: 10.1038/s41929-024-01175-8

Yao Yang, Jihan Zhou, Zipeng Zhao, Geng Sun, Saman Moniri, Colin Ophus, Yongsoo Yang, Ziyang Wei, Yakun Yuan, Cheng Zhu, Yang Liu, Qiang Sun, Qingying Jia, Hendrik Heinz, Jim Ciston, Peter Ercius, Philippe Sautet, Yu Huang, Jianwei Miao

{"title":"Atomic-scale identification of active sites of oxygen reduction nanocatalysts","authors":"Yao Yang, Jihan Zhou, Zipeng Zhao, Geng Sun, Saman Moniri, Colin Ophus, Yongsoo Yang, Ziyang Wei, Yakun Yuan, Cheng Zhu, Yang Liu, Qiang Sun, Qingying Jia, Hendrik Heinz, Jim Ciston, Peter Ercius, Philippe Sautet, Yu Huang, Jianwei Miao","doi":"10.1038/s41929-024-01175-8","DOIUrl":"10.1038/s41929-024-01175-8","url":null,"abstract":"Heterogeneous nanocatalysts play a crucial role in both the chemical and energy industries. Despite substantial advancements in theoretical, computational and experimental studies, identifying their active sites remains a major challenge. Here we utilize atomic electron tomography to determine the three-dimensional atomic structure of PtNi and Mo-doped PtNi nanocatalysts for the electrochemical oxygen reduction reaction. We then employ the experimental atomic structures as input to first-principles-trained machine learning to identify the active sites of the nanocatalysts. Through the analysis of the structure–activity relationships, we formulate an equation termed the local environment descriptor, which balances the strain and ligand effects to provide physical and chemical insights into active sites in the oxygen reduction reaction. The ability to determine the three-dimensional atomic structure and chemical composition of realistic nanoparticles, combined with machine learning, could transform our fundamental understanding of the active sites of catalysts and guide the rational design of optimal nanocatalysts. Pt-based catalysts are the state of the art for the oxygen reduction reaction. Now the three-dimensional local atomic structure of PtNi and Mo-doped PtNi nanoparticles is revealed via atomic electron tomography, and a local environment descriptor of catalytic activity is put forwards.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 7","pages":"796-806"},"PeriodicalIF":42.8,"publicationDate":"2024-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141557235","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

The solvation environment of molecularly dispersed cobalt phthalocyanine determines methanol selectivity during electrocatalytic CO2 reduction 分子分散酞菁钴的溶解环境决定了电催化二氧化碳还原过程中的甲醇选择性

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-08 DOI: 10.1038/s41929-024-01190-9

Quansong Zhu, Conor L. Rooney, Hadar Shema, Christina Zeng, Julien A. Panetier, Elad Gross, Hailiang Wang, L. Robert Baker

{"title":"The solvation environment of molecularly dispersed cobalt phthalocyanine determines methanol selectivity during electrocatalytic CO2 reduction","authors":"Quansong Zhu, Conor L. Rooney, Hadar Shema, Christina Zeng, Julien A. Panetier, Elad Gross, Hailiang Wang, L. Robert Baker","doi":"10.1038/s41929-024-01190-9","DOIUrl":"10.1038/s41929-024-01190-9","url":null,"abstract":"Heterogenized molecular electrocatalysts are a promising group of materials that can electrocatalytically convert waste molecules into higher-value products. However, how the dispersion state of molecules affects the catalytic process is not well understood. Using cobalt phthalocyanine (CoPc) dispersed on carbon nanotubes (CNTs) as a model system, here we show that increasing the direct interaction of the molecular catalyst with cations notably enhances the CO2 reduction reaction. Specifically, molecularly dispersed CoPc on CNTs yields an eightfold increase in methanol selectivity compared with aggregated CoPc on CNTs. In situ spectroscopic studies confirm the presence of two intermediates located at different positions of the double layer. Density functional theory calculations further reveal that CoPc molecules inside the Stern layer are active for methanol production due to the direct interaction with cations. Similar enhancement effects are also observed for other reactions, showing that dispersing molecular catalysts into monomeric states is a general design parameter. Heterogenized molecular catalysts provide a means to add well-defined active sites to electrode surfaces. Here, using cobalt phthalocyanine on carbon nanotubes in cation-mediated CO2 reduction, the mechanism of molecular dispersion and its impact on rate and product selectivity are revealed.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 9","pages":"987-999"},"PeriodicalIF":42.8,"publicationDate":"2024-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141557139","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