Chem Catalysis最新文献

{"title":"Reverse effect of metal-support interaction on platinum and iridium catalysts in ammonia selective oxidation","authors":"Jianhua Liu, Diru Liu, Qi An, Tingxu Chen, Yunbo Yu, Guangyan Xu, Hong He","doi":"10.1016/j.checat.2024.101229","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101229","url":null,"abstract":"Ammonia emissions from vehicles and power plants cause significant environmental concerns. Here, a range of platinum and iridium catalysts supported on oxides with various levels of reducibility were investigated in ammonia selective catalytic oxidation. Weak metal-support interaction (MSI) led to the formation of metal nanoparticles on irreducible Al₂O₃, whereas strong MSI (SMSI) induced the generation of single-atom metals on reducible CeO₂. Notably, MSI demonstrated opposite effects on the catalytic performance of Pt-based catalysts (Pt/Al₂O₃ ≫ Pt/TiO₂ > Pt/CeO₂) and Ir-based catalysts (Ir/CeO₂ > Ir/TiO₂ ≫ Ir/Al₂O₃). Metallic Pt nanoparticles on Pt/Al₂O₃ activated gaseous O₂ and promoted the low-temperature NH₃ oxidation. Conversely, on Ir/CeO₂ catalysts, the single-atom Ir-O-Ce site demonstrated high reactivity for NH₃ cleavage with an extremely low energy barrier, contributing to the superior low-temperature activity. This study provides insights into governing the MSI effect to regulate the structure on active sites of supported catalysts, thereby enhancing their catalytic performance.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"11 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858059","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}

{"title":"Key role of precatalyst composition and iron impurities in oxygen evolution reaction","authors":"Kai Zhang, Xiaohang Du, Jingde Li","doi":"10.1016/j.checat.2024.101218","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101218","url":null,"abstract":"In a recent issue of <em>Cell Reports Physical Science</em>, Bent and co-workers studied the electrochemical conversion of four typical nickel-based precatalysts toward alkaline oxygen evolution reaction and the effect of iron impurities on their conversion and catalytic activity. This is undoubtedly a key guide for designing alkaline oxygen evolution precatalysts.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"48 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849807","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}

{"title":"Enzymatic azide synthesis by ATP-dependent synthetase","authors":"Yohei Katsuyama","doi":"10.1016/j.checat.2024.101226","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101226","url":null,"abstract":"In a recent issue of <em>Nature Chemistry</em>, Zhang and coworkers showed that the ATP-dependent <em>N</em>-nitrosylase Tri17 can catalyze azide synthesis. Tri17 is a promiscuous enzyme that can catalyze <em>N</em>-nitrosylation of various substrates. When specific substrates were used, it also catalyzed the dehydration of the <em>N</em>-nitroso moiety to synthesize an azide moiety.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"12 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849831","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}

{"title":"Visualizing active species in CO2 electroreduction","authors":"Yu Yang, Yaohui Shi, Fengwang Li","doi":"10.1016/j.checat.2024.101230","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101230","url":null,"abstract":"Understanding the evolution of Cu-based catalysts during electrochemical CO₂ reduction (ECR) remains challenging. The study by Lim et al. in <em>Joule</em> devises an <em>operando</em> scanning transmission X-ray microscopy to investigate the dynamic phase transformations of Cu catalysts and reveals that Cu²⁺ species play a crucial role in enhancing C–C coupling. The findings inform the authors of an approach to dynamically redirect the oxidation state of Cu, achieving, as a result, higher selectivity and efficiency for ECR catalysis.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"31 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849762","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}

{"title":"Visualizing the step bunching on Pt surfaces and its effect in electrocatalysis with EC-STM","authors":"Zihao Zhang, Jing Guo","doi":"10.1016/j.checat.2024.101228","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101228","url":null,"abstract":"In a recent issue of <em>Nature Catalysis</em>, Rost et al. directly visualized the step bunching on flame-annealed Pt(111)-vicinal surfaces at high step densities using <em>in situ</em> electrochemical scanning tunneling microscopy (EC-STM). This phenomenon originates from the increased step-step repulsive interaction between closely distanced steps, and the surface-free energy will be lowered when forming bunched steps with wider terraces. This work challenges the common assumption that all stepped surfaces present homogeneously spaced steps of monoatomic height and provides a convincing explanation at atomic level for the anomalous electrochemical behavior of the platinum surface at high step densities, including the activity and potential of zero total charge.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"1 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849833","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}

{"title":"Decarbonizing nitrogen fertilizer production via the electrochemical nitrogen oxidation reaction","authors":"Aditya Prajapati, Alexandra Zagalskaya, Natalie Hwee, Jonathan T. Davis, Hui-Yun Jeong, Jennifer Moreno, Jenna Ynzunza, Sneha A. Akhade, Jeremy T. Feaster","doi":"10.1016/j.checat.2024.101220","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101220","url":null,"abstract":"Nitric acid is an important commodity chemical in agriculture and industry, yet its conventional production through the Haber-Bosch and Ostwald processes is energy and carbon-emission intensive. An electrochemical nitrogen oxidation reaction (NOR) to produce nitrates shows great potential as an environmentally friendly method of producing fertilizers under mild conditions. Progress in this field requires fundamental mechanistic understanding and establishing robust experimental methods, which is essential for the efficient design and synthesis of electrocatalysts for the NOR. We present a synergistic computational and experimental approach to exploring NOR pathways on a PtO&lt;sub&gt;2&lt;/sub&gt; catalyst to gain mechanistic insights into the NOR. This study marks the first attempt to perform the NOR in a vapor-fed reactor designed through advanced (additive) manufacturing. The vapor-fed reactor significantly improved the N&lt;sub&gt;2&lt;/sub&gt; mass transport to the catalyst, allowing us to report the highest rate for nitrate production to date at &lt;span&gt;&lt;span style=\"\"&gt;&lt;/span&gt;&lt;span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;mrow is=\"true\"&gt;&lt;mn is=\"true\"&gt;3.3&lt;/mn&gt;&lt;mspace width=\"0.25em\" is=\"true\" /&gt;&lt;mi is=\"true\"&gt;&amp;#x3BC;&lt;/mi&gt;&lt;mtext is=\"true\"&gt;mol&lt;/mtext&gt;&lt;mspace width=\"0.25em\" is=\"true\" /&gt;&lt;mi mathvariant=\"normal\" is=\"true\"&gt;c&lt;/mi&gt;&lt;msup is=\"true\"&gt;&lt;mi mathvariant=\"normal\" is=\"true\"&gt;m&lt;/mi&gt;&lt;mrow is=\"true\"&gt;&lt;mo is=\"true\"&gt;&amp;#x2212;&lt;/mo&gt;&lt;mn is=\"true\"&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;msup is=\"true\"&gt;&lt;mi mathvariant=\"normal\" is=\"true\"&gt;h&lt;/mi&gt;&lt;mrow is=\"true\"&gt;&lt;mo is=\"true\"&gt;&amp;#x2212;&lt;/mo&gt;&lt;mn is=\"true\"&gt;1&lt;/mn&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;/mrow&gt;&lt;/math&gt;' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"&gt;&lt;svg aria-hidden=\"true\" focusable=\"false\" height=\"2.779ex\" role=\"img\" style=\"vertical-align: -0.697ex;\" viewbox=\"0 -896.2 7838.8 1196.3\" width=\"18.206ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"&gt;&lt;g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"&gt;&lt;g is=\"true\"&gt;&lt;g is=\"true\"&gt;&lt;use xlink:href=\"#MJMAIN-33\"&gt;&lt;/use&gt;&lt;use x=\"500\" xlink:href=\"#MJMAIN-2E\" y=\"0\"&gt;&lt;/use&gt;&lt;use x=\"779\" xlink:href=\"#MJMAIN-33\" y=\"0\"&gt;&lt;/use&gt;&lt;/g&gt;&lt;g is=\"true\"&gt;&lt;/g&gt;&lt;g is=\"true\" transform=\"translate(1529,0)\"&gt;&lt;use xlink:href=\"#MJMATHI-3BC\"&gt;&lt;/use&gt;&lt;/g&gt;&lt;g is=\"true\" transform=\"translate(2133,0)\"&gt;&lt;use xlink:href=\"#MJMAIN-6D\"&gt;&lt;/use&gt;&lt;use x=\"833\" xlink:href=\"#MJMAIN-6F\" y=\"0\"&gt;&lt;/use&gt;&lt;use x=\"1334\" xlink:href=\"#MJMAIN-6C\" y=\"0\"&gt;&lt;/use&gt;&lt;/g&gt;&lt;g is=\"true\"&gt;&lt;/g&gt;&lt;g is=\"true\" transform=\"translate(3995,0)\"&gt;&lt;use xlink:href=\"#MJMAIN-63\"&gt;&lt;/use&gt;&lt;/g&gt;&lt;g is=\"true\" transform=\"translate(4440,0)\"&gt;&lt;g is=\"true\"&gt;&lt;use xlink:href=\"#MJMAIN-6D\"&gt;&lt;/use&gt;&lt;/g&gt;&lt;g is=\"true\" transform=\"translate(833,362)\"&gt;&lt;g is=\"true\"&gt;&lt;use transform=\"scale(0.707)\" xlink:href=\"#MJMAIN-2212\"&gt;&lt;/use&gt;&lt;/g&gt;&lt;g ","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"18 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841638","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}

{"title":"Photocatalytic intermolecular dearomative cycloaddition of phenanthrenes and naphthalenes with excited gem-difluoroalkenes","authors":"Yunxiao Zhang, Youyuan Guo, Yizhi Zhang, Shanshan Liu, Xiao Shen","doi":"10.1016/j.checat.2024.101200","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101200","url":null,"abstract":"Dearomative cycloaddition is a crucial method for constructing three-dimensional (3D) complex molecules from simple precursors, but the difficulty in exciting many arenes limits the application of this method. Herein, we report a photocatalytic intermolecular dearomative [2 + 2]/[4 + 2] cycloaddition of phenanthrenes and naphthalenes with excited <em>gem</em>-difluoroalkenes for the synthesis of fused <em>gem</em>-difluorocyclobutanes and <em>gem</em>-difluorocyclohexanes. Previous dearomative cycloaddition reactions involving excited phenanthrenes and naphthalenes required electron-deficient substituents to lower their excited-state energies, allowing for energy-transfer catalysis to occur. Our strategy involves excited-state <em>gem</em>-difluoroalkenes undergoing dearomative cycloaddition reactions with ground-state phenanthrenes and naphthalenes, enabling it to tolerate not only electron-deficient arenes but also electron-neutral and electron-rich arenes.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"30 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142833048","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}

{"title":"Photon-driven radical hydro-phosphoniumylation of unactivated olefins","authors":"Kaihui Liu, Chang Liu, Guangqi Hu, Tianqi Wang, Zhiyong He, Juntao Pu, Ziliang Yuan, Jing Hou, Lewu Zhan, Bindong Li, Dinghai Wang","doi":"10.1016/j.checat.2024.101219","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101219","url":null,"abstract":"Phosphonium salts are widely applied in organic synthesis, catalysis, materials science, and medicinal chemistry. Hydro-phosphoniumylation of alkene is one of the most powerful and straightforward methodologies for phosphonium salt synthesis. However, the established phospha-Michael reaction is limited to electronically activated olefins, and unactivated alkenes are not reactive. Herein, we report a photocatalytic and redox-neutral protocol for the efficient addition of phosphines and CF₃COOH to various unactivated olefins, which would be thermodynamically unfavorable under thermochemical conditions. The reaction commences with the generation of a phosphine radical cation (PRC) through the single-electron oxidation of phosphine by an excited photocatalyst. PRC adds to alkene in a kinetically barrierless manner. The method exhibits a broad substrate scope for both phosphines and alkenes. β-Deuterated phosphonium salts, whose synthesis is difficult by other methods, could also be accessed by this reaction with CF₃COOD/D₂O. Mechanistic and density functional theory (DFT) studies support a radical addition mechanism for P–C bond formation.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"41 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832690","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}

{"title":"Promoted propane dehydrogenation over Pt-In intermetallics via classic strong metal-support interaction","authors":"Ya Pan, Chunlan Qin, Ruichao Xu, Liuxin Xu, Shanshan Ruan, Xu Zhang, Kun Zheng, Xiao Han, Jinglin Yuan, Yanna Shui, Lidong Zhang, Zhihu Sun","doi":"10.1016/j.checat.2024.101198","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101198","url":null,"abstract":"The classic strong metal-support interaction (SMSI), characterized by the encapsulation of metal nanoparticles within suboxide layers, is a promising strategy for designing robust catalysts. However, applying this strategy to the high-temperature propane dehydrogenation (PDH) process, which is an important petrochemical process for the industrial production of propylene, is rarely reported. Herein, we demonstrate an SMSI-type PDH catalyst, composed of subnanometric Pt₂In₃ clusters encapsulated by an In₂O_3-<em>x</em> overlayer, exhibiting high stability and selectivity. During a 160-h on-stream test, it showed a slight activity decline (<em>k</em>_d = 0.002 h⁻¹) and maintained 99.5% propylene selectivity. The excellent performance is attributed to the dual role of the In₂O_3-<em>x</em> overlayer, which not only prevents the sintering of the Pt₂In₃ clusters but also modifies the electronic structure of Pt atoms via interfacial interaction, thus facilitating the generation and propylene desorption. Meanwhile, the Pt₂In₃ intermetallics disrupt large Pt ensembles and introduce electron-rich Pt atoms, suppressing side reactions and enhancing propylene desorption.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"32 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825752","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}

{"title":"Fe-redox-oriented electrochemical activation strategy enabling enhancement for efficient oxygen evolution reaction","authors":"Haojing Zhang, Zhaoyi Jiang, Chao Wu, Shibo Xi, Jiajia Song, Xia Long, Zhichuan J. Xu, Ye Zhou","doi":"10.1016/j.checat.2024.101196","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101196","url":null,"abstract":"Creating highly effective electrocatalysts requires understanding how materials change under varied electrochemical conditions. While much effort has been devoted to investigating structural changes under operational conditions, deliberately exposing catalysts to non-operational potential regions to electrochemically activate the catalysts and improve the catalytic performance is an underexplored area. Enlightened by the fact that Fe species exhibit pronounced redox responses in alkaline solutions within a potential range that notably falls below the oxygen evolution reaction (OER) potential region, we propose an Fe-redox-oriented electrochemical activation approach to effectively alter the catalysts’ OER performance. This approach, involving pre-cycling catalysts within the Fe-redox-rich potential range, significantly enhances the OER performance of various Fe-containing materials. For the representative Fe₃O₄@NiO catalyst, this enhancement is primarily attributed to the formation of heterojunctions and a mixed Ni-Fe surface component, which results in a more favorable electronic structure for OER.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"148 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825751","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}