Nature CatalysisPub Date : 2024-11-21DOI: 10.1038/s41929-024-01254-w
Ricardo J. Fernández-Terán
{"title":"Shining light to break planarity","authors":"Ricardo J. Fernández-Terán","doi":"10.1038/s41929-024-01254-w","DOIUrl":"10.1038/s41929-024-01254-w","url":null,"abstract":"The synthesis of rigid C(sp3)-rich isosteric mimics of heteroaromatic rings has proved a significant challenge, but is of importance in drug discovery. Now, two studies report the synthesis of densely functionalized azetidines and bicycloalkanes, using a similar concept of breaking planarity.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 11","pages":"1151-1153"},"PeriodicalIF":42.8,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679046","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}
Nature CatalysisPub Date : 2024-11-21DOI: 10.1038/s41929-024-01270-w
Francesco Zamberlan
{"title":"An enantioselective HAT for diols","authors":"Francesco Zamberlan","doi":"10.1038/s41929-024-01270-w","DOIUrl":"10.1038/s41929-024-01270-w","url":null,"abstract":"","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 11","pages":"1146-1146"},"PeriodicalIF":42.8,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679043","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}
Nature CatalysisPub Date : 2024-11-15DOI: 10.1038/s41929-024-01250-0
Wei Jie Teh, Eleonora Romeo, Shibo Xi, Ben Rowley, Francesc Illas, Federico Calle-Vallejo, Boon Siang Yeo
{"title":"Selective electroreduction of acetylene to 1,3-butadiene on iodide-induced Cuδ+–Cu0 sites","authors":"Wei Jie Teh, Eleonora Romeo, Shibo Xi, Ben Rowley, Francesc Illas, Federico Calle-Vallejo, Boon Siang Yeo","doi":"10.1038/s41929-024-01250-0","DOIUrl":"10.1038/s41929-024-01250-0","url":null,"abstract":"A crucial task towards creating a sustainable chemical industry is the electrification of chemical processes that produce value-added molecules. One such molecule is 1,3-butadiene (1,3-BD), the feedstock used for manufacturing synthetic rubber. 1,3-BD is traditionally derived, as a by-product, during the energy-intensive steam cracking of naphtha to ethylene. Here we introduce an alternative approach to selectively produce 1,3-BD from the electroreduction of acetylene (e-C2H2R). By using a potassium iodide electrolyte, we created Cuδ+–Cu0 sites on a Cu2O-nanocube-derived catalyst, which are efficacious for promoting e-C2H2R to 1,3-BD. 1,3-BD was formed with a Faradaic efficiency reaching 93% at −0.85 V versus standard hydrogen electrode (SHE) and a partial current density of −75 mA cm−2 at −1.0 V versus SHE. Density functional theory calculations show that I− preserves Cuδ+–Cu0 sites, which facilitate the favourable binding of acetylene, leading to 1,3-BD formation through the coupling of *C2H3 moieties. Electrifying energy-intensive processes is a promising approach for decarbonization. Now, 1,3-butadiene is electrochemically produced from acetylene on I−−induced Cuδ+–Cu0 sites with a Faradaic efficiency of over 90% at −0.85 VSHE and a partial current density of −75 mA cm−2 at −1.0 VSHE.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 12","pages":"1382-1393"},"PeriodicalIF":42.8,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-024-01250-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637210","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nature CatalysisPub Date : 2024-11-08DOI: 10.1038/s41929-024-01249-7
Yaguang Li, Bang Liu, Dachao Yuan, Haixiao Wang, Qixuan Wu, Yachuan Wang, Junwei Wang, Xingyuan San, Yanhong Luo, Jinhua Ye
{"title":"High-purity carbon monoxide production via photothermal formic acid decomposition over fluorite ZrO2","authors":"Yaguang Li, Bang Liu, Dachao Yuan, Haixiao Wang, Qixuan Wu, Yachuan Wang, Junwei Wang, Xingyuan San, Yanhong Luo, Jinhua Ye","doi":"10.1038/s41929-024-01249-7","DOIUrl":"10.1038/s41929-024-01249-7","url":null,"abstract":"High-purity carbon monoxide (CO), crucial for various high-tech industries, requires complex purification and further energy input. Here we show that pure fluorite ZrO2 can produce clean CO without purification by driving formic acid dehydration and completely shutting off the formic acid dehydrogenation pathway. An explosion method is developed for synthesizing pristine fluorite ZrO2 nanosheets that achieve a pure CO production rate of 55 mmol g−1 h−1 at 250 °C. Integrated with a homemade photothermal reactor, the fluorite ZrO2 nanosheets show a pure CO productivity of 83 mmol g−1 h−1 under 0.5 sun irradiation and a photochemical energy conversion efficiency of 12.3%. Moreover, this system generates over 1,538 l m−2 of pure CO per day under outdoor sunlight irradiation. This work charts a promising course for purification-free pure CO generation without secondary energy input. Obtaining high-purity CO requires energy-intensive purification processes. Here metastable fluorite ZrO2 is prepared that can catalyse thermal and photothermal formic acid dehydration to CO while completely shutting off the impurity-generating dehydrogenation pathway.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 12","pages":"1350-1358"},"PeriodicalIF":42.8,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142598074","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}
Nature CatalysisPub Date : 2024-11-01DOI: 10.1038/s41929-024-01248-8
Yigao Yuan, Jingyi Zhou, Aaron Bayles, Hossein Robatjazi, Peter Nordlander, Naomi J. Halas
{"title":"Steam methane reforming using a regenerable antenna–reactor plasmonic photocatalyst","authors":"Yigao Yuan, Jingyi Zhou, Aaron Bayles, Hossein Robatjazi, Peter Nordlander, Naomi J. Halas","doi":"10.1038/s41929-024-01248-8","DOIUrl":"10.1038/s41929-024-01248-8","url":null,"abstract":"Steam methane reforming (SMR) is the major industrial process for hydrogen production. It currently relies on high-temperature operating conditions and is associated with high carbon intensity. Photocatalytic SMR could provide greener and potentially more efficient H2 production. Here we demonstrate a plasmonic photocatalytic approach based on a Cu–Rh antenna–reactor photocatalyst for highly reactive, selective and stable SMR due to plasmon-mediated hot carrier contributions. We observe that the photocatalyst is intrinsically stable in photocatalysis but deactivates under thermocatalysis; however, the thermally deactivated catalyst can be regenerated by resonant illumination. The regeneration mechanism is studied in detail and found to be caused by plasmon-induced associative desorption of oxygen and carbon species. Catalysts used for steam methane reforming frequently suffer from deactivation by coking and oxidation. Here an active Cu–Rh plasmonic antenna–reactor photocatalyst is selective and stable under illumination but deactivates under purely thermal conditions. The thermally deactivated catalyst can then be regenerated under illumination.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 12","pages":"1339-1349"},"PeriodicalIF":42.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142561801","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}
Nature CatalysisPub Date : 2024-10-28DOI: 10.1038/s41929-024-01238-w
M. Klingenhof, H. Trzesniowski, S. Koch, J. Zhu, Z. Zeng, L. Metzler, A. Klinger, M. Elshamy, F. Lehmann, P. W. Buchheister, A. Weisser, G. Schmid, S. Vierrath, F. Dionigi, P. Strasser
{"title":"High-performance anion-exchange membrane water electrolysers using NiX (X = Fe,Co,Mn) catalyst-coated membranes with redox-active Ni–O ligands","authors":"M. Klingenhof, H. Trzesniowski, S. Koch, J. Zhu, Z. Zeng, L. Metzler, A. Klinger, M. Elshamy, F. Lehmann, P. W. Buchheister, A. Weisser, G. Schmid, S. Vierrath, F. Dionigi, P. Strasser","doi":"10.1038/s41929-024-01238-w","DOIUrl":"10.1038/s41929-024-01238-w","url":null,"abstract":"Recent efforts in anion-exchange membrane water electrolysis (AEMWE) focus on developing superior catalysts and membrane electrode assemblies to narrow the performance gaps compared with proton-exchange membrane water electrolysis (PEMWE). Here we present and characterize Ir-free AEMWE cells with NiX (X = Fe, Co or Mn) layered double hydroxide (LDH) catalyst-coated membranes with polarization characteristics and hydrogen productivities approaching those of acidic PEMWE cells, achieving >5 A cm−2 at <2.2 V. Operando spectroscopy revealed a correlation between Ni4+ centres and redox-active O ligands with an O K-edge feature, attributed to µ3-O ligands in the γ-LDH catalytic phase via density functional theory calculations. This computational–experimental study challenges the previously assumed correlation between spectral O K-edge features and oxygen evolution reaction performance in Ni-based LDH catalysts and provides insights from the molecular to the technological level demonstrating how redox-active Ni–O species and innovative catalyst-coated membrane preparation boost AEMWE performance to values rivalling state-of-the-art PEMWE cell technology. Anion-exchange membrane water electrolysers have the potential to rival more costly acidic proton-exchange membrane electrolysers, but their performance and efficiency commonly still fall short. Now an anion-exchange membrane water electrolyser is prepared with a NiFe layered double hydroxide catalyst-coated membrane that achieves high current densities above 2 A cm−2 at 1.8 V and operando X-ray absorption spectroscopy is used to track the formation of the catalytically active γ-LDH phase.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 11","pages":"1213-1222"},"PeriodicalIF":42.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519246","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}