Chinese Journal of Catalysis最新文献

{"title":"The electronic interaction of encapsulating graphene layers with FeCo alloy promotes efficient CO2 Hydrogenation to light olefins","authors":"Miao Zhang ,&nbsp;Limin Zhang ,&nbsp;Mingrui Wang ,&nbsp;Guanghui Zhang ,&nbsp;Chunshan Song ,&nbsp;Xinwen Guo","doi":"10.1016/S1872-2067(24)60188-9","DOIUrl":"10.1016/S1872-2067(24)60188-9","url":null,"abstract":"<div><h3>ABSTRACT</h3><div>CO₂ hydrogenation to value-added light olefins (C_2–4⁼) is crucial for the utilization and cycling of global carbon resource. Moderate CO₂ activation and carbon chain growth ability are key factors for iron-based catalysts for efficient CO₂ conversion to target C_2–4⁼ products. The electronic interaction and confinement effect of electron-deficient graphene inner surface on the active phase are effective to improve surface chemical properties and enhance the catalytic performance. Here, we report a core-shell FeCo alloy catalyst with graphene layers confinement prepared by a simple sol-gel method. The electron transfer from Fe species to curved graphene inner surface modifies the surface electronic structure of the active phase χ-(Fe_<em>x</em>Co_{1–<em>x</em>})₅C₂ and improves CO₂ adsorption capacity, enhancing the efficient conversion of CO₂ and moderate C-C coupling. Therefore, the catalyst FeCoK@C exhibits C_2–4⁼ selectivity of 33.0% while maintaining high CO₂ conversion of 52.0%. The high stability without obvious deactivation for over 100 h and unprecedented C_2–4⁼ space time yield (STY) up to 52.9 mmol_CO2·g^–1·h^–1 demonstrate its potential for practical application. This work provides an efficient strategy for the development of high-performance CO₂ hydrogenation catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"68 ","pages":"Pages 366-375"},"PeriodicalIF":15.7,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143094367","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}

{"title":"Recent advances in tantalum nitride for photoelectrochemical water splitting","authors":"Wenjie Yu ,&nbsp;Chao Feng ,&nbsp;Ronghua Li ,&nbsp;Beibei Zhang ,&nbsp;Yanbo Li","doi":"10.1016/S1872-2067(24)60165-8","DOIUrl":"10.1016/S1872-2067(24)60165-8","url":null,"abstract":"<div><h3>ABSTRACT</h3><div>Harnessing solar energy for renewable fuel production through artificial photosynthesis offers an ideal solution to the current energy and environmental crises. Among various methods, photoelectrochemical (PEC) water splitting stands out as a promising approach for direct solar-driven hydrogen production. Enhancing the efficiency and stability of photoelectrodes is a key focus in PEC water-splitting research. Tantalum nitride (Ta₃N₅), with its suitable band gap and band-edge positions for PEC water splitting, has emerged as a highly promising photoanode material. This review begins by introducing the history and fundamental characteristics of Ta₃N₅, emphasizing both its advantages and challenges. It then explores methods to improve light absorption efficiency, charge separation and transfer efficiency, surface reaction rate, and the stability of Ta₃N₅ photoanodes. Additionally, the review discusses the progress of research on tandem PEC cells incorporating Ta₃N₅ photoanodes. Finally, it looks ahead to future research directions for Ta₃N₅ photoanodes. The strategic approach outlined in this review can also be applied to other photoelectrode materials, providing guidance for their development.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"68 ","pages":"Pages 51-82"},"PeriodicalIF":15.7,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143094756","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}

{"title":"Orchestration of diverse components in soluble methane monooxygenase for methane hydroxylation","authors":"Yunha Hwang ,&nbsp;Dong-Heon Lee ,&nbsp;Seung Jae Lee","doi":"10.1016/S1872-2067(24)60192-0","DOIUrl":"10.1016/S1872-2067(24)60192-0","url":null,"abstract":"<div><h3>ABSTRACT</h3><div>Methane (CH₄) has a higher heat capacity (104.9 kcal/mol) than carbon dioxide (CO₂), and this has inspired research aimed at reducing methane levels to retard global warming. Hydroxylation under ambient conditions through methanotrophs can provide crucial information for understanding the harsh C–H activation of methane. Soluble methane monooxygenase (sMMO) belongs to the bacterial multi-component monooxygenase superfamily and requires hydroxylase (MMOH), regulatory (MMOB), and reductase (MMOR) components. Recent structural and biophysical studies have demonstrated that these components accelerate and retard methane hydroxylation in MMOH through protein-protein interactions. Complex structures of sMMO, including MMOH-MMOB and MMOH-MMOD, illustrate how these regulatory and inhibitory components orchestrate the di-iron active sites located within the four-helix bundles of MMOH, specifically at the docking surface known as the canyon region. In addition, recent biophysical studies have demonstrated the role of MmoR, a σ⁵⁴-dependent transcriptional regulator, in regulating sMMO expression. This perspective article introduces remarkable discoveries in recent reports on sMMO components that are crucial for understanding sMMO expression and activities. Our findings provide insight into how sMMO components interact with MMOH to control methane hydroxylation, shedding light on the mechanisms governing sMMO expression and the interactions between activating enzymes and promoters.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"68 ","pages":"Pages 204-212"},"PeriodicalIF":15.7,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143093929","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}

{"title":"Novel materials and techniques for photocatalytic water splitting developed by Professor Kazunari Domen","authors":"Yaqiang Wu ,&nbsp;Jianuo Li ,&nbsp;Wei-Kean Chong ,&nbsp;Zhenhua Pan ,&nbsp;Qian Wang","doi":"10.1016/S1872-2067(24)60152-X","DOIUrl":"10.1016/S1872-2067(24)60152-X","url":null,"abstract":"<div><h3>ABSTRACT</h3><div>Professor Kazunari Domen at the Shinshu University and the University of Tokyo has pioneered materials and techniques for solar-driven water splitting using photocatalysts, a promising technology for contributing to the construction of a sustainable and carbon-neutral society. In this paper, we summarize his groundbreaking contributions to photocatalytic water splitting and, more broadly, photocatalytic research. We highlight various novel functional photocatalytic materials, including oxides, (oxy)nitrides, and oxysulfides, along with innovative techniques such as cocatalyst engineering and Z-scheme system construction developed by the Domen Group. His team has also pioneered readily accessible and cost-effective photo(electro)chemical device fabrication methods, such as the particle-transfer method and thin-film-transfer method. Furthermore, their research has made significant contributions to understanding the (photo)catalytic mechanisms using advanced characterization techniques. Together with his research team, Professor Domen has set many milestones in the field of photocatalytic overall water splitting, notably demonstrating the first scalable and stable 100 m² solar H₂ production system using only water and sunlight. His work has revealed the potential for practical solar H₂ production from water and sunlight, and highlighted the application of fundamental principles, combined with chemical and materials science tools, to design effective photocatalytic systems. Through this review, we focus on his research and the foundational design principles that can inspire the development of efficient photocatalytic systems for water splitting and solar fuel production. By building on his contributions, we anticipate a significant impact on addressing major global energy challenges.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"68 ","pages":"Pages 1-50"},"PeriodicalIF":15.7,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143094755","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}

{"title":"Efficient nitrate electroreduction to ammonia via synergistic cascade catalysis at Cu/Fe2O3 hetero-interfaces","authors":"Xiang Zhang,&nbsp;Weihang Li,&nbsp;Jin Zhang,&nbsp;Haoshen Zhou,&nbsp;Miao Zhong","doi":"10.1016/S1872-2067(24)60194-4","DOIUrl":"10.1016/S1872-2067(24)60194-4","url":null,"abstract":"<div><h3>ABSTRACT</h3><div>Electrochemical nitrate (NO₃⁻) reduction offers a promising route for ammonia (NH₃) synthesis from industrial wastewater using renewable energy. However, achieving selective and active NO₃⁻ to NH₃ conversion at low potentials remains challenging due to complex multi-electron transfer processes and competing reactions. Herein, we tackle this challenge by developing a cascade catalysis approach using synergistic active sites at Cu-Fe₂O₃ interfaces, significantly reducing the NO₃⁻ to NH₃ at a low onset potential to about +0.4 V_RHE. Specifically, Cu optimizes *NO₃ adsorption, facilitating NO₃⁻ to nitrite (NO₂⁻) conversion, while adjacent Fe species in Fe₂O₃ promote the subsequent NO₂⁻ reduction to NH₃ with favorable *NO₂ adsorption. Electrochemical operating experiments, <em>in situ</em> Raman spectroscopy, and <em>in situ</em> infrared spectroscopy consolidate this improved onset potential and reduction kinetics <em>via</em> cascade catalysis. An NH₃ partial current density of ~423 mA cm⁻² and an NH₃ Faradaic efficiency (FE_NH3) of 99.4% were achieved at −0.6 V_RHE, with a maximum NH₃ production rate of 2.71 mmol h⁻¹ cm⁻² at −0.8 V_RHE. Remarkably, the half-cell energy efficiency exceeded 35% at −0.27 V_RHE (80% <em>i</em>R corrected), maintaining an FE_NH3 above 90% across a wide range of NO₃⁻ concentrations (0.05−1 mol L⁻¹). Using ¹⁵N isotopic tracing, we confirmed NO₃⁻ as the sole nitrogen source and attained a 98% NO₃⁻ removal efficiency. The catalyst exhibit stability over 106-h of continuous operation without noticeable degradation. This work highlights distinctive active sites in Cu-Fe₂O₃ for promoting the cascade NO₃⁻ to NO₂⁻ and NO₂⁻ to NH₃ electrolysis at industrial relevant current densities.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"68 ","pages":"Pages 404-413"},"PeriodicalIF":15.7,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143103410","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}

{"title":"Enantioselective biosynthesis of vicinal diamines enabled by synergistic photo/biocatalysis consisting of an ene-reductase and a green-light-excited organic dye","authors":"Fengming Shi ,&nbsp;Bin Chen ,&nbsp;Jinhai Yu ,&nbsp;Ruiqi Zhu ,&nbsp;Yu Zheng ,&nbsp;Xiaoqiang Huang","doi":"10.1016/S1872-2067(24)60168-3","DOIUrl":"10.1016/S1872-2067(24)60168-3","url":null,"abstract":"<div><h3>ABSTRACT</h3><div>Vicinal diamines are key motifs widely-found in many pharmaceuticals and biologically active molecules. An appealing approach for synthesizing these molecules is the amination of enamines, but few examples have been explored. With the utilization of nitrogen-centered radicals (NCRs), here we present the development of a dual bio-/photo-catalytic system for achieving enantioselective hydroamination of enamides, which can give easy access to diverse enantioenriched vicinal diamines. These reactions progress efficiently under green light excitation and exhibit excellent enantioselectivities (up to &gt;99% enantiomeric excess). Mechanistic studies uncovered the synergistic effect of the enzyme and the externally added organophotoredox catalyst Rhodamine B (RhB). This work demonstrates the effectiveness of photobiocatalysis to generate and control high-energy radical intermediates, addressing a long-standing challenge in chemical synthesis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"68 ","pages":"Pages 223-229"},"PeriodicalIF":15.7,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143093931","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}

{"title":"An unexpected reversal: The smart performance of hydrogen chloride on SbCe catalysts for NH3-SCR reaction","authors":"Caixia Liu ,&nbsp;Chaojun Huang ,&nbsp;Baiyu Fan ,&nbsp;Yan Zhang ,&nbsp;Lijing Fang ,&nbsp;Yuhe Wang ,&nbsp;Qingling Liu ,&nbsp;Weichao Wang ,&nbsp;Yanguo Chen ,&nbsp;Yawei Zhang ,&nbsp;Jiancheng Liu ,&nbsp;Fang Dong ,&nbsp;Ziyin Zhang","doi":"10.1016/S1872-2067(24)60155-5","DOIUrl":"10.1016/S1872-2067(24)60155-5","url":null,"abstract":"<div><h3>ABSTRACT</h3><div>Understanding the influence of HCl on the NH₃-selective catalytic reduction reaction mechanism is crucial for designing highly efficient denitrification catalysts. The formation of chlorate species on the surface of the synthesized SbCeO_<em>x</em> catalyst, induced by HCl, significantly enhances low-temperature activity, as evidenced by a 30% increase in NO conversion at 155 °C. Furthermore, it improves N₂ selectivity at high temperatures, with a notable 17% increase observed at 405 °C. Both experimental results and density functional theory calculations confirm that chlorate species form at Ce sites. This formation facilitates the creation of oxygen vacancies, boosting the oxygen exchange capacity. It also increases NH₃ adsorption at the Ce sites, promotes the formation of Sb-OH, and reduces competitive OH adsorption on these sites. Notably, compared with the reaction mechanism without HCl, the presence of chlorate species enhances NH₃ adsorption and activation, which is vital for subsequent catalytic reactions.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"68 ","pages":"Pages 376-385"},"PeriodicalIF":15.7,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143094369","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}

{"title":"4d Metal-doped liquid Ga for efficient ammonia electrosynthesis at wide N2 concentrations","authors":"Yingying Wei,&nbsp;Yuyao Sun,&nbsp;Yaodong Yu,&nbsp;Yue Shi,&nbsp;Zhe Wu,&nbsp;Lei Wang,&nbsp;Jianping Lai","doi":"10.1016/S1872-2067(24)60144-0","DOIUrl":"10.1016/S1872-2067(24)60144-0","url":null,"abstract":"<div><div>Electrocatalytic nitrogen reduction reaction under ambient conditions is a promising pathway for ammonia synthesis. Currently nitrogen reduction reactions are carried out in N₂-saturated environments and use high-purity nitrogen as feedstock, which is costly. Here, we prepared carbon-coated ultra-low 4<em>d</em> metal Ru-doped liquid metal Ga (Ru_0.06/LM@C) for NRR over a wide range of N₂ concentrations. Comprehensive analyses show that the introduction of the ultra-low 4<em>d</em> element Ru can effectively adjust the electronic structure through orbital interactions, thus enhancing the adsorption of nitrogen-containing intermediates. The liquid catalyst utilized its mobility to provide a higher density of active sites. In addition, the material Ru_0.06/Ga@C itself has the ability to promote product desorption. The three act synergistically to optimize the N₂ mass transfer path, thereby increasing the *NNH coverage and further improving the ammonia yield over a wide range of N₂ concentrations. The maximum NH₃ yield of the catalyst can reach 126.0 μg h⁻¹ mg_cat⁻¹ (at –0.3 V <em>vs</em>. RHE) with high purity N₂ as feed gas, and the Faraday efficiency is 60.4% at –0.1 V <em>vs</em>. RHE. Over a wide range of N₂ concentrations, the NH₃ yield of the catalyst was greater than 100 μg h⁻¹ mg_cat⁻¹ with a Faraday efficiency higher than 47%. The catalytic performance is much higher than that of solid Ga@C and reported <em>p</em>-block metal-based catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 194-203"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143170972","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}

{"title":"Site-selective benzylic C–H oxidation through mediated electrolysis","authors":"Yi-Fan Xi ,&nbsp;Rui-Xing Gao ,&nbsp;Ping Fang ,&nbsp;Ya-Ping Han ,&nbsp;Cong Ma ,&nbsp;Tian-Sheng Mei","doi":"10.1016/S1872-2067(24)60139-7","DOIUrl":"10.1016/S1872-2067(24)60139-7","url":null,"abstract":"<div><div>A novel strategy for site-selective benzylic C–H oxidation has been developed through mediated electrolysis. A bulky maleimide <em>N</em>-oxyl radical (MINO) generated by proton-coupled electrochemical oxidation of <em>N</em>-hydroxymaleimide (NHMI), serves as a hydrogen atom-transfer mediator. Good-to-excellent site selectivity was observed among different substrates, providing a practical approach for site-selective benzylic C–H oxidation. Additionally, the hydrogen-atom transfer mechanism for C–H electrochemical oxidation allows the oxidation to proceed at much lower anode potentials relative to direct electrolysis and with minimal reliance on the substrate's electronic properties.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 54-60"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143172203","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}

{"title":"Role of extra-framework aluminum species within MOR zeolites for syngas conversion via OXZEO catalysis","authors":"Haodi Wang ,&nbsp;Feng Jiao ,&nbsp;Jingyao Feng ,&nbsp;Yuting Sun ,&nbsp;Guangjin Hou ,&nbsp;Xiulian Pan ,&nbsp;Xinhe Bao","doi":"10.1016/S1872-2067(24)60135-X","DOIUrl":"10.1016/S1872-2067(24)60135-X","url":null,"abstract":"<div><div>The location of aluminum within the framework or extra-framework of zeolites is a critical factor in determining its catalytic performance. Despite extensive research on the identification and formation mechanism of extra-framework aluminum (EFAl), its impact on catalytic performance requires further investigation. Herein, mordenite (MOR) zeolites with comparable acid density within the 8MR and 12MR channels but different EFAl contents were prepared, and their catalytic roles were examined in syngas conversion. Intelligent gravimetric analysis, model experiment of ethylene conversion and thermogravimetric analysis demonstrate that the existence of EFAl species can inhibit the secondary conversion of ethylene to long chain hydrocarbons (i.e., C₅₊) as well as the over-accumulation of carbonaceous species. However, excessive EFAl species lead to rapid deactivation due to restricted space and thus severe diffusion limitation. MOR zeolite with a moderate amount of EFAl species achieves a superior ethylene selectivity and exhibits an enhanced stability in syngas conversion when combined with ZnAlO_<em>x</em> oxide. The insights gained in this work provide important guidance for the design of more efficient zeolite-based catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"67 ","pages":"Pages 135-143"},"PeriodicalIF":15.7,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143170975","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}