Chinese Journal of Catalysis最新文献

{"title":"Nickel nanoparticles catalyzed hydrogenation and deuteration for a general amine synthesis","authors":"Xiaofei Wang ,&nbsp;Yan Li ,&nbsp;Mengyun Wang,&nbsp;Yiming Gao,&nbsp;Zhuang Ma,&nbsp;Aiwen Lei,&nbsp;Wu Li","doi":"10.1016/S1872-2067(25)64658-4","DOIUrl":"10.1016/S1872-2067(25)64658-4","url":null,"abstract":"<div><div>Amines represent fundamental motifs in various chemical contexts and are widely used in agrochemicals and pharmaceuticals. The development of earth-abundant metal-based heterogeneous catalysts for the synthesis amines remains an important goal in terms of chemical research and industrial application/manufacture. Herein, we developed an efficient and highly selective nitrogen-doped nickel catalyst enriched with Lewis acid sites, which has been applied for to the hydrogenative coupling of nitriles and amines with molecular hydrogen for the synthesis of a train of functionalised and structurally diverse secondary and tertiary amines. Furthermore, catalytic hydrogenation and deuteration of nitriles were achieved under milder conditions, yielding a series of primary amines and deuterated amines with high deuterium incorporation.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 392-401"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106085","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":"In-situ Pt reduction induced topological transformation of NiFe-MOF for industrial seawater splitting","authors":"Guohao Na ,&nbsp;Hongshun Zheng ,&nbsp;Mingpeng Chen ,&nbsp;Huachuan Sun ,&nbsp;Yuewen Wu ,&nbsp;Dequan Li ,&nbsp;Yun Chen ,&nbsp;Boran Zhao ,&nbsp;Bo Zhao ,&nbsp;Tong Zhou ,&nbsp;Tianwei He ,&nbsp;Yuxiao Zhang ,&nbsp;Jianhong Zhao ,&nbsp;Yumin Zhang ,&nbsp;Jin Zhang ,&nbsp;Feng Liu ,&nbsp;Hao Cui ,&nbsp;Qingju Liu","doi":"10.1016/S1872-2067(24)60271-8","DOIUrl":"10.1016/S1872-2067(24)60271-8","url":null,"abstract":"<div><div>Metal-support interaction (MSI) is regarded as an indispensable manner to stabilize active metals and modulate catalytic activity, which shows great potentials in developing of efficient hydrogen evolution reaction (HER) electrode with high activity and strong robustness. Herein, this work presents a novel heterostructure with ultrafine platinum quantum dots (Pt QDs) on defective catalytic supports derived from metal-organic frameworks (MOFs). It is indicated substantial oxygen vacancies can be generated and Pt–Pt bonds can be optimized through topological transformation. The resulting Pt/T-NiFe-BDC (BDC: C₈H₆O₄) exhibits competitive HER activity in alkaline seawater, attaining ultralow overpotentials of 158 and 266 mV at 500 and 1000 mA cm^–2 with fast kinetics and outstanding stability. An asymmetric water electrolyzer using Pt/T-NiFe-BDC as a cathode only requires a voltage of 1.89 V to generate an industrial density of 1000 mA cm^–2 and shows no attenuation in 500-h continuous test at 500 mA cm^–2. Theoretical calculations and <em>in-situ</em> spectroscopic analysis reveal the reversible hydrogen spillover mechanism, in which oxygen vacancies facilitate the sluggish water dissociation and Pt QDs promote the H* combination. This study provides a new paradigm to engineer metal-supported catalysts for efficient and robust seawater splitting.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 211-221"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106185","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":"Engineering d-p hybridization in Ni-Bx cocatalysts for superior photocatalytic H2 evolution efficiency","authors":"Junjiang Zhu ,&nbsp;Xiaofang Li","doi":"10.1016/S1872-2067(24)60684-5","DOIUrl":"10.1016/S1872-2067(24)60684-5","url":null,"abstract":"","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 1-3"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106193","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":"S-scheme g-C3N4/BiOBr heterojunction for efficient photocatalytic H2O2 production","authors":"Tengfei Cao ,&nbsp;Quanlong Xu ,&nbsp;Jun Zhang ,&nbsp;Shenggao Wang ,&nbsp;Tingmin Di ,&nbsp;Quanrong Deng","doi":"10.1016/S1872-2067(24)60277-9","DOIUrl":"10.1016/S1872-2067(24)60277-9","url":null,"abstract":"<div><div>The establishment of S-scheme heterojunctions has arisen as a promising strategy for the advancement of efficient photocatalytic systems with superior charge separation and redox ability, specifically for H₂O₂ production. In this investigation, an innovative 2D/2D g-C₃N₄/BiOBr S-scheme heterojunction was meticulously engineered through an <em>in situ</em> growth methodology. The synthetic composites exhibit boosted H₂O₂ production activity, achieving a peak generation rate of 392 μmol L^–1 h^–1, approximately 8.7-fold and 2.1-fold increase over the pristine BiOBr and g-C₃N₄, respectively. Such a superior activity should be attributed to the highly efficient charge separation and migration mechanisms, along with the sustained robust redox capability of S-scheme heterostructure, which are verified by time-resolved photoluminescence spectroscopy, photocurrent test and electron paramagnetic resonance measurements. Furthermore, the interfacial electric field induced S-scheme charge transfer mechanism between g-C₃N₄ and BiOBr is systematically certificated by <em>in situ</em> irradiated X-ray photoelectron spectroscopy and density functional theory calculation. This research offers a comprehensive protocol for the systematic development and construction of highly efficient S-scheme heterojunction photocatalysts, specifically tailored for enhanced H₂O₂ production.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 118-129"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106265","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":"Ultra-high overpotential induces NiS2 deep reconstruction to significantly improve HER performance","authors":"Chao Feng ,&nbsp;Jiaxin Shao ,&nbsp;Hanyang Wu ,&nbsp;Afaq Hassan ,&nbsp;Hengpan Yang ,&nbsp;Jiaying Yu ,&nbsp;Qi Hu ,&nbsp;Chuanxin He","doi":"10.1016/S1872-2067(24)60286-X","DOIUrl":"10.1016/S1872-2067(24)60286-X","url":null,"abstract":"<div><div>It is well known that transition metal sulfides (TMS) (i.e., NiS₂) undergo electrochemical reconstructions to generate highly active Ni₃S₂ during the process of hydrogen evolution reaction (HER) under overpotentials of &lt; 500 mV. However, at higher overpotentials, Ni₃S₂ can theoretically be further restructured into Ni and thus form Ni/Ni₃S₂ heterogeneous interface structures, which may provide opportunities to further enhance HER activity of NiS₂. Here, we selected NiS₂ as a model electrocatalyst and investigated the influence of the reconstruction results induced from regular to ultrahigh overpotentials on its electrocatalytic hydrogen precipitation performance. The experimental results showed that the most significant enhancement of hydrogen precipitation performance was obtained for the NiS₂@CC-900 (900 means 900 mV overpotential) sample after the ultra-high overpotential induced reconstruction. Compared with the initial overpotential of 161 mV (10 mA cm^–2), the overpotential of the reconstructed sample reduced by 67 mV (42%). The characterization results showed that an ultra-high overpotential of 900 mV induced deep reconstruction of NiS₂, formed highly reactive Ni/Ni₃S₂ heterogeneous interfaces, which is more conducive to improved HER performance and match well with theoretical calculations results. We demonstrated ultrahigh overpotential was an effective strategy to induce NiS₂ deeply reconstruction and significantly improve its HER performance, and this strategy was also applicable to CoS₂ and FeS₂. This study provides an extremely simple and universal pathway for the reasonable construction of efficient electrocatalysts by induced TMS deeply reconstruction.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 230-242"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106189","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":"Unsaturated cobalt single-atoms stabilized by silanol nests of zeolites for efficient propane dehydrogenation","authors":"Liwen Guo ,&nbsp;Dao Shi ,&nbsp;Tianjun Zhang ,&nbsp;Yanhang Ma ,&nbsp;Guodong Qi ,&nbsp;Jun Xu ,&nbsp;Qiming Sun","doi":"10.1016/S1872-2067(25)64660-2","DOIUrl":"10.1016/S1872-2067(25)64660-2","url":null,"abstract":"<div><div>Propane dehydrogenation (PDH) has emerged as a key on-purpose technology for the production of propylene, but it often depends on toxic chromium and expensive platinum catalysts, highlighting the need for environmentally friendly and cost-effective alternatives. In this study, we developed a facile impregnation method to fabricate unsaturated Co single-atoms with a tricoordinated Co₁O₃H_<em>x</em> structure by regulating silanol nests in purely siliceous Beta zeolites. Detailed PDH catalytic tests and characterizations revealed a positive correlation between the presence of silanol nests and enhanced catalytic activity. Additionally, the unsaturated Co single-atoms exhibited a carbon deposition rate more than an order of magnitude slower than that of Co nanoparticles. Notably, the optimized Co_0.3%/deAl-meso-Beta catalyst achieved a record-high propylene formation rate of 21.2 mmol_C3H6 g_cat^–1 h^–1, with an exceptional propylene selectivity of 99.1% at 550 °C. Moreover, the Co_0.3%/deAl-meso-Beta catalyst demonstrated excellent stability, with negligible deactivation after 5 consecutive regeneration cycles. This study emphasizes the pivotal role of silanol nests of zeolites in stabilizing and modulating the coordination environment of metallic active sites, providing valuable insights for the design of high-activity, high-stability, and low-cost PDH catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 323-333"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106080","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":"Interfacial engineering of a plasmonic Ag/Ag2CO3/C3N5 S-scheme heterojunction for high-performance photocatalytic degradation of antibiotics","authors":"Shijie Li ,&nbsp;Xinyu Li ,&nbsp;Yanping Liu ,&nbsp;Peng Zhang ,&nbsp;Junlei Zhang ,&nbsp;Bin Zhang","doi":"10.1016/S1872-2067(25)64652-3","DOIUrl":"10.1016/S1872-2067(25)64652-3","url":null,"abstract":"<div><div>Devising S-scheme heterostructure is considered as a cutting-edge strategy for advanced photocatalysts with effectively segregated photo-carriers and prominent redox potential for emerging organic pollutants control. Herein, an S-scheme Ag₂CO₃/C₃N₅ heterojunction photocatalyst was developed via a simple in situ chemical deposition procedure, and further photoreduction operation made metallic Ag (size: 3.5–12.5 nm) being in situ formed on Ag₂CO₃/C₃N₅ for a plasmonic S-scheme Ag/Ag₂CO₃/C₃N₅ heterojunction photocatalyst. Consequently, Ag/Ag₂CO₃/C₃N₅ manifests pronouncedly upgraded photocatalytic performance toward oxytetracycline degradation with a superior photoreaction rate constant of 0.0475 min^‒1, which is 13.2, 3.9 and 2.2 folds that of C₃N₅, Ag₂CO₃, and Ag₂CO₃/C₃N₅, respectively. As evidenced by comprehensive characterizations and density functional theory calculations, the localized surface plasmon resonance effect of metallic Ag and the unique S-scheme charge transfer mechanism in 0D/0D/2D Ag/Ag₂CO₃/C₃N₅ collaboratively strengthen the visible-light absorption, and facilitate the effective separation of powerful charge carriers, thereby significantly promoting the generation of reactive species like <strong>·</strong>OH^–, h⁺ and <strong>·</strong>O₂^– for efficient oxytetracycline destruction. Moreover, four consecutive cycles demonstrate the reusability of Ag/Ag₂CO₃/C₃N₅. Furthermore, the authentic water purification tests affirm its practical application potential. This work not only provides a candidate strategy for advancing S-scheme heterojunction photocatalysts but also makes a certain contribution to water decontamination.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 130-142"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106180","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":"Active non-bonding oxygen mediate lattice oxygen oxidation on NiFe2O4 achieving efficient and stable water oxidation","authors":"Jiangyu Tang ,&nbsp;Xiao Wang ,&nbsp;Yunfa Wang ,&nbsp;Min Shi ,&nbsp;Peng Huo ,&nbsp;Jianxiang Wu ,&nbsp;Qiaoxia Li ,&nbsp;Qunjie Xu","doi":"10.1016/S1872-2067(24)60276-7","DOIUrl":"10.1016/S1872-2067(24)60276-7","url":null,"abstract":"<div><div>The oxygen evolution reaction (OER) serves as a fundamental half–reaction in the electrolysis of water for hydrogen production, which is restricted by the sluggish OER reaction kinetics and unable to be practically applied. The traditional lattice oxygen oxidation mechanism (LOM) offers an advantageous route by circumventing the formation of M-OOH* in the adsorption evolution mechanism (AEM), thus enhancing the reaction kinetics of the OER but resulting in possible structural destabilization due to the decreased M–O bond order. Fortunately, the asymmetry of tetrahedral and octahedral sites in transition metal spinel oxides permits the existence of non-bonding oxygen, which could be activated by rational band structure design for direct O-O coupling, where the M–O bond maintains its initial bond order. Here, non-bonding oxygen was introduced into NiFe₂O₄ <em>via</em> annealing in an oxygen-deficient atmosphere. Then, <em>in-situ</em> grown sulfate species on octahedral nickel sites significantly improved the reactivity of the non-bonding oxygen electrons, thereby facilitating the transformation of the redox center from metal to oxygen. LOM based on non-bonding oxygen (LOM_NB) was successfully activated within NiFe₂O₄, exhibiting a low overpotential of 206 mV to achieve a current density of 10 mA cm^–2 and excellent durability of stable operation for over 150 h. Additionally, catalysts featuring varying band structures were synthesized for comparative analysis, and it was found that the reversible redox processes of non-bonding oxygen and the accumulation of non-bonding oxygen species containing 2<em>p</em> holes are critical prerequisites for triggering and sustaining the LOM_NB pathway in transition metal spinel oxides. These findings may provide valuable insights for the future development of spinel-oxide-based LOM catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 164-175"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106183","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":"Unveiling complexities: Reviews on insights into the mechanism of oxygen evolution reaction","authors":"Pengxiang Zhang ,&nbsp;Jiawen Wang ,&nbsp;Tianyu Yang ,&nbsp;Ruizhe Wang ,&nbsp;Ruofan Shen ,&nbsp;Zhikun Peng ,&nbsp;Yanyan Liu ,&nbsp;Xianli Wu ,&nbsp;Jianchun Jiang ,&nbsp;Baojun Li","doi":"10.1016/S1872-2067(25)64653-5","DOIUrl":"10.1016/S1872-2067(25)64653-5","url":null,"abstract":"<div><div>The study of the oxygen evolution reaction (OER) mechanism is vital for advancing our understanding of this pivotal energy conversion process. This review synthesizes recent advancements in OER mechanism, emphasizing the intricate relationship between catalytic mechanisms and catalyst design. This review discusses the connotation and cutting-edge progress of traditional mechanisms such as adsorbate evolution mechanism (AEM) and lattice oxygen mechanism (LOM) as well as emerging pathways including oxide path mechanism (OPM), oxo-oxo coupling mechanism (OCM), and intramolecular oxygen coupling mechanism (IMOC) etc. Innovative research progress on the coexistence and transformation of multiple mechanisms is highlighted, and the intrinsic factors that influence these dynamic processes are summarized. Advanced characterization techniques and theoretical modeling are underscored as indispensable tools for revealing these complex interactions. This review provides guiding principles for mechanism-based catalyst design. Finally, in view of the multidimensional challenges currently faced by OER mechanisms, prospects for future research are given to bridge the gap between mechanism innovation and experimental verification and application. This comprehensive review provides valuable perspectives for advancing clean energy technologies and achieving sustainable development.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 48-83"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144105656","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":"Unveiling the catalytic active sites of iron-vanadium catalysts for the selective oxidation of methanol to formaldehyde","authors":"Yujie Zhan ,&nbsp;Chengqin Zhong ,&nbsp;Mingli Bi ,&nbsp;Yafei Liang ,&nbsp;Yuji Qi ,&nbsp;Jiaqi Chen ,&nbsp;Jiaxu Liu ,&nbsp;Xindang Zhang ,&nbsp;Shuai Zhang ,&nbsp;Yehong Wang ,&nbsp;Feng Wang","doi":"10.1016/S1872-2067(24)60279-2","DOIUrl":"10.1016/S1872-2067(24)60279-2","url":null,"abstract":"<div><div>Iron-Vanadium (FeV) catalyst showed a unique catalytic activity for the selective oxidation of methanol to formaldehyde; however, due to its complex compositions, the identification of catalytic active sites still remains challenging, inhibiting the rational design of excellent FeV-based catalysts. Here, in this work, a series of FeV catalysts with various compositions, including FeVO₄, isolated VO_<em>x</em>, low-polymerized V_<em>n</em>O_<em>x</em>, and crystalline V₂O₅ were prepared by controlling the preparation conditions, and were applied to methanol oxidation to formaldehyde reaction. A FeV_1.1 catalyst, which consisted of FeVO₄ and low-polymerized V_<em>n</em>O_<em>x</em> species showed an excellent catalytic performance with a methanol conversion of 92.3% and a formaldehyde selectivity of 90.6%, which was comparable to that of conventional iron-molybdate catalyst. The results of CH₃OH-IR, O₂ pulse and control experiments revealed a crucial synergistic effect between FeVO₄ and low-polymerized V_<em>n</em>O_<em>x</em>. It enhanced the oxygen supply capacity and suitable binding and adsorption strengths for formaldehyde intermediates, contributing to the high catalytic activity and formaldehyde selectivity. This study not only advances the understanding of FeV structure but also offers valuable guidelines for selective methanol oxidation to formaldehyde.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 334-343"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106081","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}