Pub Date : 2024-04-23DOI: 10.1038/s41929-024-01150-3
Manu Suvarna, Javier Pérez-Ramírez
Accelerating catalyst discovery and development is of paramount importance in addressing the global energy, sustainability and healthcare demands. The past decade has witnessed significant momentum in harnessing data science concepts in catalysis research to aid the aforementioned cause. Here we comprehensively review how catalysis practitioners have leveraged data-driven strategies to solve complex challenges across heterogeneous, homogeneous and enzymatic catalysis. We delineate all studies into deductive or inductive modes, and statistically infer the prevalence of catalytic tasks, model reactions, data representations and choice of algorithms. We highlight frontiers in the field and knowledge transfer opportunities among the catalysis subdisciplines. Our critical assessment reveals a glaring gap in data science exploration in experimental catalysis, which we bridge by elaborating on four pillars of data science, namely descriptive, predictive, causal and prescriptive analytics. We advocate their adoption into routine experimental workflows and underscore the importance of data standardization to spur future research in digital catalysis. The use of data science tools in catalysis research has experienced a surge in the past 10–15 years. This Review provides a holistic overview and categorization of the field across the various approaches and subdisciplines in catalysis.
{"title":"Embracing data science in catalysis research","authors":"Manu Suvarna, Javier Pérez-Ramírez","doi":"10.1038/s41929-024-01150-3","DOIUrl":"10.1038/s41929-024-01150-3","url":null,"abstract":"Accelerating catalyst discovery and development is of paramount importance in addressing the global energy, sustainability and healthcare demands. The past decade has witnessed significant momentum in harnessing data science concepts in catalysis research to aid the aforementioned cause. Here we comprehensively review how catalysis practitioners have leveraged data-driven strategies to solve complex challenges across heterogeneous, homogeneous and enzymatic catalysis. We delineate all studies into deductive or inductive modes, and statistically infer the prevalence of catalytic tasks, model reactions, data representations and choice of algorithms. We highlight frontiers in the field and knowledge transfer opportunities among the catalysis subdisciplines. Our critical assessment reveals a glaring gap in data science exploration in experimental catalysis, which we bridge by elaborating on four pillars of data science, namely descriptive, predictive, causal and prescriptive analytics. We advocate their adoption into routine experimental workflows and underscore the importance of data standardization to spur future research in digital catalysis. The use of data science tools in catalysis research has experienced a surge in the past 10–15 years. This Review provides a holistic overview and categorization of the field across the various approaches and subdisciplines in catalysis.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":42.8,"publicationDate":"2024-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140635953","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}
Pub Date : 2024-04-23DOI: 10.1038/s41929-024-01152-1
Javier Corpas, Henry P. Caldora, Ester Maria Di Tommaso, Augusto César Hernandez-Perez, Oliver Turner, Luis Miguel Azofra, Alessandro Ruffoni, Daniele Leonori
The introduction of alkylamines onto heteroaromatics is integral to the preparation of high-value molecules. Typical methods rely on heteroaromatic pre-functionalization by halogenation or nitration, followed by metal-catalysed cross-coupling or multi-step manipulation of the nitrogen functionality. This results in often unselective or low-yielding synthetic routes. Here we show an alternative approach in which saturated heterocyclic ketones are used as aryl surrogates for desaturative coupling with amines. The process operates under mild photochemical conditions, is compatible with complex amines and delivers both electron-poor and -rich heteroaromatics that are difficult to access by other methods. As ketones are readily decorated by carbonyl chemistry, this retrosynthetic tactic escapes the rules and limitations of aromatic reactivity and metal-catalysed cross-couplings. Our process uses enamine formation to create the key carbon–nitrogen bond, followed by two rounds of photoredox oxidation and cobalt-catalysed desaturation. The two desaturation steps are distinct, as the cobaloxime first acts as a hydrogen atom abstractor and then an oxidant. Aminated heteroaromatics are usually synthesized from heteroaromatic substrates. Now, a general photochemical approach that exploits non-aromatic N-heterocyclic ketones as starting materials for the coupling with amines under desaturative catalysis is reported as an alternative.
{"title":"A general strategy for the amination of electron-rich and electron-poor heteroaromatics by desaturative catalysis","authors":"Javier Corpas, Henry P. Caldora, Ester Maria Di Tommaso, Augusto César Hernandez-Perez, Oliver Turner, Luis Miguel Azofra, Alessandro Ruffoni, Daniele Leonori","doi":"10.1038/s41929-024-01152-1","DOIUrl":"10.1038/s41929-024-01152-1","url":null,"abstract":"The introduction of alkylamines onto heteroaromatics is integral to the preparation of high-value molecules. Typical methods rely on heteroaromatic pre-functionalization by halogenation or nitration, followed by metal-catalysed cross-coupling or multi-step manipulation of the nitrogen functionality. This results in often unselective or low-yielding synthetic routes. Here we show an alternative approach in which saturated heterocyclic ketones are used as aryl surrogates for desaturative coupling with amines. The process operates under mild photochemical conditions, is compatible with complex amines and delivers both electron-poor and -rich heteroaromatics that are difficult to access by other methods. As ketones are readily decorated by carbonyl chemistry, this retrosynthetic tactic escapes the rules and limitations of aromatic reactivity and metal-catalysed cross-couplings. Our process uses enamine formation to create the key carbon–nitrogen bond, followed by two rounds of photoredox oxidation and cobalt-catalysed desaturation. The two desaturation steps are distinct, as the cobaloxime first acts as a hydrogen atom abstractor and then an oxidant. Aminated heteroaromatics are usually synthesized from heteroaromatic substrates. Now, a general photochemical approach that exploits non-aromatic N-heterocyclic ketones as starting materials for the coupling with amines under desaturative catalysis is reported as an alternative.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140636082","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}
Pub Date : 2024-04-23DOI: 10.1038/s41929-024-01137-0
Michael A. Reiter, Timothy Bradley, Lars A. Büchel, Philipp Keller, Emese Hegedis, Thomas Gassler, Julia A. Vorholt
Methanol synthesized from captured greenhouse gases is an emerging renewable feedstock with great potential for bioproduction. Recent research has raised the prospect of methanol bioconversion to value-added products using synthetic methylotrophic Escherichia coli, as its metabolism can be rewired to enable growth solely on the reduced one-carbon compound. Here we describe the generation of an E. coli strain that grows on methanol at a doubling time of 4.3 h—comparable to many natural methylotrophs. To establish bioproduction from methanol using this synthetic chassis, we demonstrate biosynthesis from four metabolic nodes from which numerous bioproducts can be derived: lactic acid from pyruvate, polyhydroxybutyrate from acetyl coenzyme A, itaconic acid from the tricarboxylic acid cycle and p-aminobenzoic acid from the chorismate pathway. In a step towards carbon-negative chemicals and valorizing greenhouse gases, our work brings synthetic methylotrophy in E. coli within reach of industrial applications. Synthetic methylotrophic organisms provide potential for valorization of greenhouse gas-derived methanol. Here an Escherichia coli strain is generated that reaches a similar growth rate on methanol to many natural methylotrophs and is capable of producing chemicals from this carbon source.
从捕获的温室气体中合成的甲醇是一种新兴的可再生原料，具有巨大的生物生产潜力。最近的研究提出了利用人工合成的滋养甲基大肠杆菌将甲醇生物转化为高附加值产品的前景，因为大肠杆菌的新陈代谢可以重新连接，使其只在还原一碳化合物上生长。在这里，我们描述了一种大肠杆菌菌株的产生过程，这种菌株在甲醇上生长的加倍时间为 4.3 小时，与许多天然的养甲菌相当。为了利用这种合成底盘从甲醇中建立生物生产，我们展示了四个代谢节点的生物合成过程，从中可以衍生出多种生物产品：丙酮酸产生的乳酸、乙酰辅酶 A 产生的多羟基丁酸、三羧酸循环产生的衣康酸以及络氨酸途径产生的对氨基苯甲酸。我们的工作使大肠杆菌中的合成甲营养体进入了工业应用领域，为实现负碳化学品和温室气体的价值化迈出了一步。
{"title":"A synthetic methylotrophic Escherichia coli as a chassis for bioproduction from methanol","authors":"Michael A. Reiter, Timothy Bradley, Lars A. Büchel, Philipp Keller, Emese Hegedis, Thomas Gassler, Julia A. Vorholt","doi":"10.1038/s41929-024-01137-0","DOIUrl":"10.1038/s41929-024-01137-0","url":null,"abstract":"Methanol synthesized from captured greenhouse gases is an emerging renewable feedstock with great potential for bioproduction. Recent research has raised the prospect of methanol bioconversion to value-added products using synthetic methylotrophic Escherichia coli, as its metabolism can be rewired to enable growth solely on the reduced one-carbon compound. Here we describe the generation of an E. coli strain that grows on methanol at a doubling time of 4.3 h—comparable to many natural methylotrophs. To establish bioproduction from methanol using this synthetic chassis, we demonstrate biosynthesis from four metabolic nodes from which numerous bioproducts can be derived: lactic acid from pyruvate, polyhydroxybutyrate from acetyl coenzyme A, itaconic acid from the tricarboxylic acid cycle and p-aminobenzoic acid from the chorismate pathway. In a step towards carbon-negative chemicals and valorizing greenhouse gases, our work brings synthetic methylotrophy in E. coli within reach of industrial applications. Synthetic methylotrophic organisms provide potential for valorization of greenhouse gas-derived methanol. Here an Escherichia coli strain is generated that reaches a similar growth rate on methanol to many natural methylotrophs and is capable of producing chemicals from this carbon source.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-024-01137-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140636211","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}
Pub Date : 2024-04-22DOI: 10.1038/s41929-024-01131-6
Cong Tian, Roham Dorakhan, Joshua Wicks, Zhu Chen, Kyoung-Shin Choi, Nirala Singh, Joshua A. Schaidle, Adam Holewinski, Aleksandra Vojvodic, Dionisios G. Vlachos, Linda J. Broadbelt, Edward H. Sargent
Biomass incorporates carbon captured from the atmosphere and can serve as a renewable feedstock for producing valuable chemicals and fuels. Here we look at how electrochemical approaches can impact biomass valorization, focusing on identifying chemical transformations that leverage renewable electricity and feedstocks to produce valorized products via electro-privileged transformations. First, we recommend that the field should explore widening the spectrum of platform chemicals derived from bio-feedstocks, thus offering pathways to molecules that have historically been derived from petroleum. Second, we identify opportunities in electrocatalytic production of energy-dense fuels from biomass that utilize water as the hydrogen source and renewable electricity as the driving force. Finally, we look at the potential in electrochemical depolymerization to preserve key functional groups in raw feedstocks that would otherwise be lost during harsh pre-treatments in traditional depolymerization routes. On the basis of these priorities, we suggest a roadmap for the integration of biomass and electrochemistry and offer milestones required to tap further into the potential of electrochemical biomass valorization. Biomass is a renewable source of carbon that can be exploited to produce valuable chemicals and fuels. This Perspective discusses the electrochemical valorization of biomass, identifying specific chemical transformations in which the approach can excel.
{"title":"Progress and roadmap for electro-privileged transformations of bio-derived molecules","authors":"Cong Tian, Roham Dorakhan, Joshua Wicks, Zhu Chen, Kyoung-Shin Choi, Nirala Singh, Joshua A. Schaidle, Adam Holewinski, Aleksandra Vojvodic, Dionisios G. Vlachos, Linda J. Broadbelt, Edward H. Sargent","doi":"10.1038/s41929-024-01131-6","DOIUrl":"10.1038/s41929-024-01131-6","url":null,"abstract":"Biomass incorporates carbon captured from the atmosphere and can serve as a renewable feedstock for producing valuable chemicals and fuels. Here we look at how electrochemical approaches can impact biomass valorization, focusing on identifying chemical transformations that leverage renewable electricity and feedstocks to produce valorized products via electro-privileged transformations. First, we recommend that the field should explore widening the spectrum of platform chemicals derived from bio-feedstocks, thus offering pathways to molecules that have historically been derived from petroleum. Second, we identify opportunities in electrocatalytic production of energy-dense fuels from biomass that utilize water as the hydrogen source and renewable electricity as the driving force. Finally, we look at the potential in electrochemical depolymerization to preserve key functional groups in raw feedstocks that would otherwise be lost during harsh pre-treatments in traditional depolymerization routes. On the basis of these priorities, we suggest a roadmap for the integration of biomass and electrochemistry and offer milestones required to tap further into the potential of electrochemical biomass valorization. Biomass is a renewable source of carbon that can be exploited to produce valuable chemicals and fuels. This Perspective discusses the electrochemical valorization of biomass, identifying specific chemical transformations in which the approach can excel.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140632153","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}
Molecular metal complex catalysts are highly tunable in terms of their CO2 reduction performance by means of their flexible molecular design. However, metal complex catalysts have challenges in their structural stability and it has not been possible to synthesize high-value-added C3 products due to their inability to perform C–C coupling. Here we show a CO2 reduction reaction catalysed by a Br-bridged dinuclear Cu(I) complex that produces C3H7OH with high robustness during the reaction. The C–C coupling reaction mechanism was analysed by experimental operando surface-enhanced Raman scattering analysis, and theoretical quantum-chemical calculations proposed the formation of a C–C coupling intermediate species with substrate incorporation between the two Cu centres. Molecular design guidelines based on this discovery offer an approach to developing next-generation catalysts that generate multicarbon CO2 reduction products. The tunable design of molecular catalysts presents opportunities for the control of product selectivity in CO2 reduction, yet to date, complexes capable of producing multicarbon products have been elusive. Here, a Br-bridged dinuclear Cu(I) complex that turns over C3H7OH is reported.
分子金属络合催化剂通过灵活的分子设计，可对其二氧化碳还原性能进行高度调整。然而，金属络合物催化剂在结构稳定性方面存在挑战，而且由于其无法进行 C-C 偶联，因此一直无法合成高附加值的 C3 产物。在此，我们展示了一种由桥桥双核 Cu(I) 复合物催化的 CO2 还原反应，该反应在反应过程中能产生 C3H7OH，且具有很高的稳定性。我们通过实验操作表面增强拉曼散射分析分析了 C-C 耦合反应机理，并通过量子化学理论计算提出了在两个 Cu 中心之间形成底物结合的 C-C 耦合中间产物。基于这一发现的分子设计指南为开发生成多碳二氧化碳还原产物的下一代催化剂提供了一种方法。
{"title":"Dinuclear Cu(I) molecular electrocatalyst for CO2-to-C3 product conversion","authors":"Naonari Sakamoto, Keita Sekizawa, Soichi Shirai, Takamasa Nonaka, Takeo Arai, Shunsuke Sato, Takeshi Morikawa","doi":"10.1038/s41929-024-01147-y","DOIUrl":"10.1038/s41929-024-01147-y","url":null,"abstract":"Molecular metal complex catalysts are highly tunable in terms of their CO2 reduction performance by means of their flexible molecular design. However, metal complex catalysts have challenges in their structural stability and it has not been possible to synthesize high-value-added C3 products due to their inability to perform C–C coupling. Here we show a CO2 reduction reaction catalysed by a Br-bridged dinuclear Cu(I) complex that produces C3H7OH with high robustness during the reaction. The C–C coupling reaction mechanism was analysed by experimental operando surface-enhanced Raman scattering analysis, and theoretical quantum-chemical calculations proposed the formation of a C–C coupling intermediate species with substrate incorporation between the two Cu centres. Molecular design guidelines based on this discovery offer an approach to developing next-generation catalysts that generate multicarbon CO2 reduction products. The tunable design of molecular catalysts presents opportunities for the control of product selectivity in CO2 reduction, yet to date, complexes capable of producing multicarbon products have been elusive. Here, a Br-bridged dinuclear Cu(I) complex that turns over C3H7OH is reported.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-024-01147-y.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140556728","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}
Understanding the structural evolution of individual active sites during a reaction is a long-standing target in surface science and catalysis. It is still challenging to precisely characterize in situ the intrinsic nature and evolution of the active site because the active site is too small for characterization techniques to decipher the local properties. Here we used electrochemical tip-enhanced Raman spectroscopy to monitor the geometric and electronic evolution of individual active sites of MoS2 during the hydrogen evolution reaction. Reconstruction regions of 40 nm with varied lattice and electron density from the edge to the nearby basal plane were observed during the hydrogen evolution reaction. We further revealed the progressive generation of active sites during the activation process. The synergistic reconstruction around edge due to the lattice deformation reduces the activation energy barriers and promotes the electrocatalytic reaction. These discoveries offer insights into our understanding of the active site and its dynamics during electrocatalysis. Electrocatalysts are often dynamic and their surface structure changes under working conditions. Now the dynamic evolution of MoS2 edges is monitored with nanometre-resolution via electrochemical tip-enhanced Raman spectroscopy during the hydrogen evolution reaction.
{"title":"Visualizing the structural evolution of individual active sites in MoS2 during electrocatalytic hydrogen evolution reaction","authors":"Teng-Xiang Huang, Xin Cong, Si-Si Wu, Jiang-Bin Wu, Yi-Fan Bao, Mao-Feng Cao, Liwen Wu, Miao-Ling Lin, Xiang Wang, Ping-Heng Tan, Bin Ren","doi":"10.1038/s41929-024-01148-x","DOIUrl":"10.1038/s41929-024-01148-x","url":null,"abstract":"Understanding the structural evolution of individual active sites during a reaction is a long-standing target in surface science and catalysis. It is still challenging to precisely characterize in situ the intrinsic nature and evolution of the active site because the active site is too small for characterization techniques to decipher the local properties. Here we used electrochemical tip-enhanced Raman spectroscopy to monitor the geometric and electronic evolution of individual active sites of MoS2 during the hydrogen evolution reaction. Reconstruction regions of 40 nm with varied lattice and electron density from the edge to the nearby basal plane were observed during the hydrogen evolution reaction. We further revealed the progressive generation of active sites during the activation process. The synergistic reconstruction around edge due to the lattice deformation reduces the activation energy barriers and promotes the electrocatalytic reaction. These discoveries offer insights into our understanding of the active site and its dynamics during electrocatalysis. Electrocatalysts are often dynamic and their surface structure changes under working conditions. Now the dynamic evolution of MoS2 edges is monitored with nanometre-resolution via electrochemical tip-enhanced Raman spectroscopy during the hydrogen evolution reaction.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":42.8,"publicationDate":"2024-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140556802","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}
Pub Date : 2024-04-12DOI: 10.1038/s41929-024-01136-1
Xuepeng Zhong, Lijun Sui, Menghao Yang, Toshinari Koketsu, Malte Klingenhof, Sören Selve, Kyle G. Reeves, Chuangxin Ge, Lin Zhuang, Wang Hay Kan, Maxim Avdeev, Miao Shu, Nicolas Alonso-Vante, Jin-Ming Chen, Shu-Chih Haw, Chih-Wen Pao, Yu-Chung Chang, Yunhui Huang, Zhiwei Hu, Peter Strasser, Jiwei Ma
The design of materials that efficiently catalyse the electrochemical reaction of molecular oxygen to hydroxide ions is key to the development of electrochemical devices. Here we demonstrate an approach to control the orbital hybridization of 3d and 4d/5d metals to tune the adsorption strength and stabilize the catalytic sites in the platinum-free catalysts Li2Mn1−xRuxO3. We show that in these materials, the stabilization of O 2p holes by changing the M–O covalency (M = 4d/5d metal) can help to mitigate structural instability. Operando X-ray absorption spectroscopy revealed that the Mn and Ru atoms are the active sites for the oxygen reduction reaction (ORR) and exhibit a high ORR activity with noteworthy stability compared with the Pt/C catalyst and outperform NiFe layered double hydroxides and RuO2 in the oxygen evolution reaction. Notably, Li2Mn0.85Ru0.15O3 shows a high power density of 1.2 W cm−2 and current density of 1.2 A cm−2 at 1.9 V in the anion exchange membrane fuel cell and water electrolyser, respectively. The development of superior and cost-effective catalysts for the oxygen reduction and evolution reactions is pivotal for the future hydrogen economy. Now a series of Ru-modified Li2MnO3 catalysts have been designed to optimize the electronic structure and achieve a high performance in both oxygen reduction and evolution reactions, as demonstrated in practical anion exchange membrane fuel cell and water electrolyser tests.
设计能有效催化分子氧到氢氧根离子电化学反应的材料是开发电化学设备的关键。在这里，我们展示了一种控制 3d 和 4d/5d 金属轨道杂化的方法，以调整无铂催化剂 Li2Mn1-xRuxO3 中的吸附强度并稳定催化位点。我们的研究表明，在这些材料中，通过改变 M-O 共价（M = 4d/5d 金属）来稳定 O 2p 孔有助于缓解结构的不稳定性。运算X射线吸收光谱显示，Mn和Ru原子是氧还原反应（ORR）的活性位点，与Pt/C催化剂相比，它们具有较高的ORR活性和显著的稳定性，在氧进化反应中的性能优于NiFe层状双氢氧化物和RuO2。值得注意的是，在阴离子交换膜燃料电池和水电解槽中，Li2Mn0.85Ru0.15O3 在 1.9 V 电压下的功率密度和电流密度分别高达 1.2 W cm-2 和 1.2 A cm-2。
{"title":"Stabilization of layered lithium-rich manganese oxide for anion exchange membrane fuel cells and water electrolysers","authors":"Xuepeng Zhong, Lijun Sui, Menghao Yang, Toshinari Koketsu, Malte Klingenhof, Sören Selve, Kyle G. Reeves, Chuangxin Ge, Lin Zhuang, Wang Hay Kan, Maxim Avdeev, Miao Shu, Nicolas Alonso-Vante, Jin-Ming Chen, Shu-Chih Haw, Chih-Wen Pao, Yu-Chung Chang, Yunhui Huang, Zhiwei Hu, Peter Strasser, Jiwei Ma","doi":"10.1038/s41929-024-01136-1","DOIUrl":"10.1038/s41929-024-01136-1","url":null,"abstract":"The design of materials that efficiently catalyse the electrochemical reaction of molecular oxygen to hydroxide ions is key to the development of electrochemical devices. Here we demonstrate an approach to control the orbital hybridization of 3d and 4d/5d metals to tune the adsorption strength and stabilize the catalytic sites in the platinum-free catalysts Li2Mn1−xRuxO3. We show that in these materials, the stabilization of O 2p holes by changing the M–O covalency (M = 4d/5d metal) can help to mitigate structural instability. Operando X-ray absorption spectroscopy revealed that the Mn and Ru atoms are the active sites for the oxygen reduction reaction (ORR) and exhibit a high ORR activity with noteworthy stability compared with the Pt/C catalyst and outperform NiFe layered double hydroxides and RuO2 in the oxygen evolution reaction. Notably, Li2Mn0.85Ru0.15O3 shows a high power density of 1.2 W cm−2 and current density of 1.2 A cm−2 at 1.9 V in the anion exchange membrane fuel cell and water electrolyser, respectively. The development of superior and cost-effective catalysts for the oxygen reduction and evolution reactions is pivotal for the future hydrogen economy. Now a series of Ru-modified Li2MnO3 catalysts have been designed to optimize the electronic structure and achieve a high performance in both oxygen reduction and evolution reactions, as demonstrated in practical anion exchange membrane fuel cell and water electrolyser tests.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140547975","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}
Pub Date : 2024-04-11DOI: 10.1038/s41929-024-01154-z
Jian Li, Xin Mu, Wenyue Dong, Yun Chen, Qianjin Kang, Guang Zhao, Jin Hou, Ramon Gonzalez, Linquan Bai, Yan Feng, Chen Yang, Tiangang Liu, Zaigao Tan
{"title":"Author Correction: A non-carboxylative route for the efficient synthesis of central metabolite malonyl-CoA and its derived products","authors":"Jian Li, Xin Mu, Wenyue Dong, Yun Chen, Qianjin Kang, Guang Zhao, Jin Hou, Ramon Gonzalez, Linquan Bai, Yan Feng, Chen Yang, Tiangang Liu, Zaigao Tan","doi":"10.1038/s41929-024-01154-z","DOIUrl":"10.1038/s41929-024-01154-z","url":null,"abstract":"","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-024-01154-z.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140651222","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}
Pub Date : 2024-04-09DOI: 10.1038/s41929-024-01134-3
Ádám Balog, Egon Kecsenovity, Gergely F. Samu, Jie He, Dávid Fekete, Csaba Janáky
Photoelectrochemistry holds the promise of directly converting sunlight to valuable chemical products. Photoelectrochemical (PEC) methods, however, lag behind their electrochemical counterparts in terms of current density. In this work, we demonstrate that, by using concentrated sunlight, we can achieve current densities similar to electrochemical methods, but with lower energy input. Specifically, we combined the direct PEC oxidation of glycerol with the dark hydrogen evolution or CO2 reduction in a membrane-separated continuous-flow PEC cell. We achieved over 110 mA cm−2 photocurrent density, which is at least an order of magnitude larger than those typically reported in the literature. We demonstrated that the product distribution of glycerol oxidation is notably different in PEC and electrochemical scenarios at the same current density, and the parasitic oxygen evolution reaction can be suppressed in the PEC case. This approach raises opportunities to drive complex electrochemical reactions in a more selective manner. Photoelectrocatalysis offers the potential to reduce energy demand and provide different selectivity profiles compared with electrocatalytic analogues, but current systems have shown limited rates. Here, recent advances in light concentration and gas diffusion electrodes are integrated into a photoelectrochemical system for coupled glycerol oxidation and CO2/H2O reduction with photocurrent densities above 100 mA cm−2.
{"title":"Paired photoelectrochemical conversion of CO2/H2O and glycerol at high rate","authors":"Ádám Balog, Egon Kecsenovity, Gergely F. Samu, Jie He, Dávid Fekete, Csaba Janáky","doi":"10.1038/s41929-024-01134-3","DOIUrl":"10.1038/s41929-024-01134-3","url":null,"abstract":"Photoelectrochemistry holds the promise of directly converting sunlight to valuable chemical products. Photoelectrochemical (PEC) methods, however, lag behind their electrochemical counterparts in terms of current density. In this work, we demonstrate that, by using concentrated sunlight, we can achieve current densities similar to electrochemical methods, but with lower energy input. Specifically, we combined the direct PEC oxidation of glycerol with the dark hydrogen evolution or CO2 reduction in a membrane-separated continuous-flow PEC cell. We achieved over 110 mA cm−2 photocurrent density, which is at least an order of magnitude larger than those typically reported in the literature. We demonstrated that the product distribution of glycerol oxidation is notably different in PEC and electrochemical scenarios at the same current density, and the parasitic oxygen evolution reaction can be suppressed in the PEC case. This approach raises opportunities to drive complex electrochemical reactions in a more selective manner. Photoelectrocatalysis offers the potential to reduce energy demand and provide different selectivity profiles compared with electrocatalytic analogues, but current systems have shown limited rates. Here, recent advances in light concentration and gas diffusion electrodes are integrated into a photoelectrochemical system for coupled glycerol oxidation and CO2/H2O reduction with photocurrent densities above 100 mA cm−2.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-024-01134-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140538694","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：