Chinese Journal of Catalysis最新文献_第3页

Defective UiO-66(Ce) supported Ni nanoparticles with optimized microenvironment and electronic state for efficient olefin hydrogenation reaction 缺陷的UiO-66（Ce）负载镍纳米颗粒具有优化的微环境和电子态，用于高效的烯烃加氢反应

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-05-01 DOI: 10.1016/S1872-2067(24)60284-6

Rushuo Li , Tao Ban , Danfeng Zhao , Fajie Hu , Jing Lin , Xiubing Huang , Zhiping Tao , Ge Wang

{"title":"Defective UiO-66(Ce) supported Ni nanoparticles with optimized microenvironment and electronic state for efficient olefin hydrogenation reaction","authors":"Rushuo Li , Tao Ban , Danfeng Zhao , Fajie Hu , Jing Lin , Xiubing Huang , Zhiping Tao , Ge Wang","doi":"10.1016/S1872-2067(24)60284-6","DOIUrl":"10.1016/S1872-2067(24)60284-6","url":null,"abstract":"<div><div>Defect engineering improves the catalytic performance of metal-organic frameworks (MOFs) loaded metal nanoparticles (MNPs@MOFs), but there is still a challenge in defining the structure-activity relationships. Herein, the content of linker-missing defects in UiO-66(Ce) was systematically regulated via formic acid as the modulators, and defective UiO-66(Ce) loaded Ni nanoparticles (NPs) were constructed for dicyclopentadiene (DCPD) hydrogenation. The fine regulation of defect engineering and reduction conditions affected the structure properties of UiO-66(Ce) and the electronic metal-support interaction between MOFs and Ni NPs, thereby optimizing the microenvironment and electronic state of Ni NPs. The optimized U(Ce)-40eq with suitable defects, small size and structure stability effectively promoted the production of highly dispersed abundant electron-deficient Ni<sup>0</sup> active sites, enhancing the adsorption and activation of H<sub>2</sub> and C=C bonds, especially accelerating the rate-determining step. Therefore, U(Ce)-40eq loaded 5 wt% Ni NPs achieved DCPD saturated hydrogenation to tetrahydrodicyclopentadiene (70 °C, 2 MPa, 90 min), superior to most high-loading Ni-based catalysts. This work reveals the synergistic mechanism of MOFs defect engineering and electronic structure of Ni NPs, providing effective guidance for the precise preparation of highly efficient and stable MNPs@MOFs heterogeneous catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 344-358"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106082","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}

引用次数: 0

Boost proton transfer in water oxidation by constructing local electric fields on BiVO4 photoanodes 在BiVO4光阳极上构建局部电场促进水氧化过程中的质子转移

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-05-01 DOI: 10.1016/S1872-2067(25)64665-1

Zhixing Guan , Ying Zhang , Fangfang Feng , Zhaohui Li , Yanli Liu , Zifeng Wu , Xingxing Zheng , Xionghui Fu , Yuanming Zhang , Wenbin Liao , Jialu Chen , Hongguang Liu , Yi Zhu , Yongge Wei

{"title":"Boost proton transfer in water oxidation by constructing local electric fields on BiVO4 photoanodes","authors":"Zhixing Guan , Ying Zhang , Fangfang Feng , Zhaohui Li , Yanli Liu , Zifeng Wu , Xingxing Zheng , Xionghui Fu , Yuanming Zhang , Wenbin Liao , Jialu Chen , Hongguang Liu , Yi Zhu , Yongge Wei","doi":"10.1016/S1872-2067(25)64665-1","DOIUrl":"10.1016/S1872-2067(25)64665-1","url":null,"abstract":"<div><div>The slow-proton-fast-electron process severely limits the catalytic efficiency of oxygen evolution reaction. A method is proposed to accelerate proton transfer by building up local electric fields. Modifying acetic, ethanedioic and propanetricarboxylic (C<sub>6</sub>H<sub>8</sub>O<sub>6</sub>) ligands on BiVO<sub>4</sub> surface results in a potential difference between BiVO<sub>4</sub> and ligands that generates a local electric field which serves as a driving force for proton transfer. Among the ligands, carrying the strongest electron-withdrawing ability, the modification of C<sub>6</sub>H<sub>8</sub>O<sub>6</sub> forms the strongest local electric field and leads to the fastest proton transfer and the smallest thermodynamic overpotential. C<sub>6</sub>H<sub>8</sub>O<sub>6</sub>-BiVO<sub>4</sub> exhibits 3.5 times photocurrent density as high as that of pure BiVO<sub>4</sub>, which is 3.50 mA cm<sup>–2</sup> at 1.23 V<sub>RHE</sub>. The onset potential of C<sub>6</sub>H<sub>8</sub>O<sub>6</sub>-BiVO<sub>4</sub> shifts negatively from 0.70 to 0.38 V<sub>RHE</sub>. The mechanism for OER transitions from thermodynamically high energy proton-coupled electron transfer to thermodynamically low energy electron transfer as proton transfer is accelerated.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 176-186"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106182","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}

引用次数: 0

Peripheral NV-induced electron transfer to Fe1 single atoms for highly efficient O2 activation 外周nv诱导电子转移到Fe1单原子，以实现高效的O2活化

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-05-01 DOI: 10.1016/S1872-2067(25)64651-1

Fenli Liu , Man Yang , Jianglin Duan , Zhiyu Yin , Mingyang Shi , Fuqing Chen , Huifeng Xiong , Xin Liu , Wengang Liu , Qixing Xia , Shaodong Sun , Dan Feng , Haifeng Qi , Yong Qin , Yujing Ren

{"title":"Peripheral NV-induced electron transfer to Fe1 single atoms for highly efficient O2 activation","authors":"Fenli Liu , Man Yang , Jianglin Duan , Zhiyu Yin , Mingyang Shi , Fuqing Chen , Huifeng Xiong , Xin Liu , Wengang Liu , Qixing Xia , Shaodong Sun , Dan Feng , Haifeng Qi , Yong Qin , Yujing Ren","doi":"10.1016/S1872-2067(25)64651-1","DOIUrl":"10.1016/S1872-2067(25)64651-1","url":null,"abstract":"<div><div>Catalytic oxidation plays a crucial role in chemical industry, in which the utilization of abundant and environmental-friendly oxygen (O<sub>2</sub>) as oxidant aligns with sustainable development principles in green chemistry. However, the intrinsic inertness of ground-state O<sub>2</sub> molecule poses a long-standing challenge in developing an efficient non-noble metal-based catalyst. Herein, inspired by the electron transfer process in respiratory chain, we engineered long-range N<sub>V</sub> to mediate Fe<sub>1</sub> center for O<sub>2</sub> activation in aerobic oxidation. Combined in/quasi-situ spectroscopic characterizations and control experiments suggest the Fe<sub>1</sub> site efficiently adsorbs O<sub>2</sub>, and the N<sub>V</sub> site facilitates electron delocalization to adjacent Fe<sub>1</sub>, providing efficient transformation of O<sub>2</sub> to reactive oxygen species that boost oxidation reactions mildly. This Fe<sub>1</sub>–N<sub>V</sub> single-atom catalyst demonstrates outstanding catalytic performance in aerobic oxidations of alkanes, N-heterocycles, alcohols, and amines under relatively mild conditions. Our findings offer a new perspective for designing high-efficiency heterogeneous catalysts in aerobic oxidations, promising various potential applications.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 187-198"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106184","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}

引用次数: 0

Impregnation of ionic liquid into porous Fe-N-C electrocatalyst to improve electrode kinetics and mass transport for polymer electrolyte fuel cells 离子液体浸渍多孔Fe-N-C电催化剂以改善聚合物电解质燃料电池的电极动力学和质量传递

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-05-01 DOI: 10.1016/S1872-2067(25)64654-7

Siming Li , Enyang Sun , Pengfei Wei , Wei Zhao , Suizhu Pei , Ying Chen , Jie Yang , Huili Chen , Xi Yin , Min Wang , Yawei Li

{"title":"Impregnation of ionic liquid into porous Fe-N-C electrocatalyst to improve electrode kinetics and mass transport for polymer electrolyte fuel cells","authors":"Siming Li , Enyang Sun , Pengfei Wei , Wei Zhao , Suizhu Pei , Ying Chen , Jie Yang , Huili Chen , Xi Yin , Min Wang , Yawei Li","doi":"10.1016/S1872-2067(25)64654-7","DOIUrl":"10.1016/S1872-2067(25)64654-7","url":null,"abstract":"<div><div>Developing efficient and stable non-precious metal catalysts is essential for replacing platinum-based catalysts in polymer electrolyte membrane fuel cells (PEMFCs). The transition metal and nitrogen co-doped carbon electrocatalyst (M-N-C) is considered an effective alternative to precious metal catalysts. However, its relatively poor performance in acidic environments has always been a problem plaguing its practical application in PEMFCs. This study presents a sequential deposition methodology for constructing a composite catalytic system of Fe-N-C and ionic liquid (IL), which exhibits improved performance at both half-cell and membrane electrode assembly scales. The presence of IL significantly inhibits H<sub>2</sub>O<sub>2</sub> production, preferentially promoting the 4e<sup>–</sup> O<sub>2</sub> reduction reaction, resulting in improved electrocatalytic activity and stability. Additionally, the enhanced PEMFC performance of IL containing electrodes is a direct result of the improved ionic and reactant accessibility of the pore confined Fe-N-C catalysts where the IL minimizes local resistive transport losses. This study establishes a strategic foundation for the practical utilization of non-precious metal catalysts in PEMFCs and other energy converting technologies.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 277-288"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106072","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}

引用次数: 0

Crystal facet engineering of Bi2O2CO3 nanosheets to enhance photocatalytic ozonation: Unraveling ozone adsorption and electron transfer mechanism 增强光催化臭氧氧化作用的Bi2O2CO3纳米片晶面工程：揭示臭氧吸附和电子转移机制

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-05-01 DOI: 10.1016/S1872-2067(24)60270-6

Yang Yang , Zhou Yang , Zhiming Lai , Can Yang , Yidong Hou , Huilin Tao , Jinshui Zhang , Masakazu Anpo , Xianzhi Fu

{"title":"Crystal facet engineering of Bi2O2CO3 nanosheets to enhance photocatalytic ozonation: Unraveling ozone adsorption and electron transfer mechanism","authors":"Yang Yang , Zhou Yang , Zhiming Lai , Can Yang , Yidong Hou , Huilin Tao , Jinshui Zhang , Masakazu Anpo , Xianzhi Fu","doi":"10.1016/S1872-2067(24)60270-6","DOIUrl":"10.1016/S1872-2067(24)60270-6","url":null,"abstract":"<div><div>Photocatalytic ozonation holds promise for advanced water purification, yet its development has been hindered by a limited understanding of ozone activation mechanisms and its related photogenerated electron transfer dynamics. Herein, we employed in-situ DRIFTS and Raman spectroscopy to elucidate the distinct adsorption and activation behaviors of ozone (O<sub>3</sub>) on the {001} and {110} crystal facets of Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub> (BOC) nanosheets. BOC-{001} demonstrates superior photocatalytic ozonation performance, with 85% phenol mineralization and excellent durability, significantly outperforming the 53% mineralization rate of BOC-{110}. This enhanced activity is attributed to non-dissociative ozone adsorption and favorable adsorption energy over {001} facet, which facilitate the one-electron O<sub>3</sub> reduction pathway. Furthermore, crystal facet engineering strengthens the built-in electric field, promoting exciton dissociation and the generation of localized charge carriers. The synergistic effects of optimized electron availability and ozone adsorption significantly boost the production of reactive oxygen species. These findings provide a deeper understanding of the critical roles of O<sub>3</sub> adsorption and electron transfer in radical generation, which could provide some guidance for the strategic development of highly effective photocatalytic ozonation catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 143-153"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106266","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}

引用次数: 0

Programmed protein scaffold for multienzyme assembly empowering the biosynthesis of rare sugars 用于多酶组装的程序化蛋白质支架，赋予稀有糖的生物合成能力

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-05-01 DOI: 10.1016/S1872-2067(25)64675-4

Xin Gao , Guangyao Tang , Jiajun Yan , Senbiao Fang , Kangming Tian , Fuping Lu , Hui-Min Qin

{"title":"Programmed protein scaffold for multienzyme assembly empowering the biosynthesis of rare sugars","authors":"Xin Gao , Guangyao Tang , Jiajun Yan , Senbiao Fang , Kangming Tian , Fuping Lu , Hui-Min Qin","doi":"10.1016/S1872-2067(25)64675-4","DOIUrl":"10.1016/S1872-2067(25)64675-4","url":null,"abstract":"<div><div>Multienzyme cascades enable the sequential synthesis of complex chemicals by combining multiple catalytic processes in one pot, offering considerable time and cost savings compared to a series of separate batch reactions. However, challenges related to coordination and regulatory interplay among multiple enzymes reduce the catalytic efficiency of such cascades. Herein, we genetically programmed a scaffold framework that selectively and orthogonally recruits enzymes as designed. The system was then used to generate multienzyme complexes of D-allulose 3-epimerase (DAE), ribitol dehydrogenase (RDH), and formate dehydrogenase (FDH) for rare sugar production. This scaffolded multienzymatic assembly achieves a 10.4-fold enhancement in the catalytic performance compared to its unassembled counterparts, obtaining allitol yield of more than 95%. Molecular dynamics simulations revealed that shorter distances between neighboring enzymes in scaffold-mounted complexes facilitated the transfer of reaction intermediates. A dual-module catalytic system incorporating (1) scaffold-bound complexes of DAE, RDH, and FDH and (2) scaffold-bound complexes of alcohol dehydrogenase and NADH oxidase expressed intracellularly in <em>E. coli</em> was used to synthesize D-allulose from D-fructose. This system synthesized 90.6% D-allulose from 300 g L<sup>−1</sup> D-fructose, with a space-time yield of 13.6 g L<sup>−1</sup> h<sup>−1</sup>. Our work demonstrates the programmability and versatility of scaffold-based strategies for the advancement of multienzyme cascades.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 95-105"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144105658","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}

引用次数: 0

Single-atomic Fe sites modulated by Sn regulator for enhanced electrochemical CO2 reduction 用Sn调节剂调制单原子铁位增强电化学CO2还原

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-05-01 DOI: 10.1016/S1872-2067(24)60269-X

Chenghong Hu , Yue Zhang , Yi Zhang, Qintong Huang, Kui Shen, Liyu Chen, Yingwei Li

{"title":"Single-atomic Fe sites modulated by Sn regulator for enhanced electrochemical CO2 reduction","authors":"Chenghong Hu , Yue Zhang , Yi Zhang, Qintong Huang, Kui Shen, Liyu Chen, Yingwei Li","doi":"10.1016/S1872-2067(24)60269-X","DOIUrl":"10.1016/S1872-2067(24)60269-X","url":null,"abstract":"<div><div>Single-atom Fe catalysts show significant promise in the electrocatalytic reduction of CO<sub>2</sub> (CO<sub>2</sub>RR), while their performance remains inferior to that of precious metal catalysts due to the overly strong binding of *CO intermediates. Although the introduction of heteroatoms or transition metal sites can modulate the binding strength of *CO on Fe sites, these regulators often induce competitive hydrogen evolution reaction (HER) with reduced Faraday efficiency (FE). In this work, we employ HER-inert Sn as a regulator to tune the electronic structure of Fe, weakening *CO adsorption and enhancing CO<sub>2</sub>RR performance. Diatomic Fe-Sn pairs supported on N-doped carbon (Fe-Sn/NC) were synthesized, achieving FE for CO exceeding 90% over a broad potential range from −0.4 to −0.9 V versus the reversible hydrogen electrode. Fe-Sn/NC shows a high turnover frequency of 1.5 × 10<sup>4</sup> h<sup>−1</sup>, much higher than that of Fe/NC. Characterization results and theoretical calculations demonstrate that bonding Sn site to Fe generates electron-rich Fe centers, effectively reducing the adsorption strength of *CO without triggering HER. Additionally, Fe-Sn/NC exhibits exceptional activity in hydrazine oxidation performance (HzOR). The HzOR-assisted CO<sub>2</sub>RR system using Fe-Sn/NC as electrodes reduces energy consumption by 38% compared with the conventional CO<sub>2</sub>RR coupled oxygen evolution reaction system.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 222-229"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106187","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}

引用次数: 0

Boosting charge transfer at inorganic/organic S-scheme interface for photo-Fenton degradation of antibiotics and bacterial inactivation 促进无机/有机S-scheme界面电荷转移的光- fenton降解抗生素和细菌灭活

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-05-01 DOI: 10.1016/S1872-2067(24)60265-2

Haotian Qin , Yuxin Huang , Qiang Cheng, Suding Yan, Kai Wang

{"title":"Boosting charge transfer at inorganic/organic S-scheme interface for photo-Fenton degradation of antibiotics and bacterial inactivation","authors":"Haotian Qin , Yuxin Huang , Qiang Cheng, Suding Yan, Kai Wang","doi":"10.1016/S1872-2067(24)60265-2","DOIUrl":"10.1016/S1872-2067(24)60265-2","url":null,"abstract":"<div><div>Solar-driven Fenton-like reactions are promising strategies for degrading pharmaceutical wastewater to address environmental challenges and antibiotic pollution. However, its efficacy is limited by suboptimal light absorption efficiency, rapid charge recombination, and inadequate interfacial charge transfer. In this study, an inorganic/organic S-scheme photo-Fenton system of pseudobrookite/carbon nitride (FTOCN) was synthesized <em>via</em> a hydrothermally coupled calcination process for the effective purification of tetracycline antibiotics under visible-light irradiation. The optimized FTOCN-2 heterostructure exhibits a significantly enhanced TC degradation capacity of 90% within 60 min. The rate constant of FTOCN-2 is 1.6 and 5.2 times greater than those of FTO and CN, respectively. Furthermore, FTOCN exhibits high antibacterial efficacy, highlighting its potential application in the purification of natural water. Measurements <em>via</em> a range of analytical techniques, including Kelvin probe force microscopy, density functional theory calculations, <em>in situ</em> X-ray photoelectron spectroscopy, and femtosecond transient absorption spectroscopy, corroborate the S-scheme mechanism. This study provides a novel perspective for the development of photo-Fenton systems with S-scheme heterojunctions for water purification.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 106-117"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144105659","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}

引用次数: 0

Boosting the Volmer step by synergistic coupling of dilute CuRu nanoalloy with Cu/Ru dual single atoms for efficient and CO-tolerant alkaline hydrogen oxidation 稀cuu纳米合金与Cu/Ru双单原子的协同耦合提高了Volmer步长，实现了高效耐co的碱性氢氧化

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-05-01 DOI: 10.1016/S1872-2067(25)64670-5

Yi Liu , Shuqing Zhou , Chenggong Niu , Tayirjan Taylor Isimjan , Yongfa Zhu , Dingsheng Wang , Xiulin Yang , Jieshan Qiu , Bin Wu

{"title":"Boosting the Volmer step by synergistic coupling of dilute CuRu nanoalloy with Cu/Ru dual single atoms for efficient and CO-tolerant alkaline hydrogen oxidation","authors":"Yi Liu , Shuqing Zhou , Chenggong Niu , Tayirjan Taylor Isimjan , Yongfa Zhu , Dingsheng Wang , Xiulin Yang , Jieshan Qiu , Bin Wu","doi":"10.1016/S1872-2067(25)64670-5","DOIUrl":"10.1016/S1872-2067(25)64670-5","url":null,"abstract":"<div><div>Active and poisoning-resistant Ru-based electrocatalysts for the hydrogen oxidation reaction (HOR) are designed and fabricated by integrating Cu/Ru dual single atoms and alloy CuRu nanoparticles (N-(CuRu)<sub>NP+SA</sub>@NC) through a strategy involving weak chemical reduction and ammonia-assisted gas-phase nitridation. The resultant N-(CuRu)<sub>NP+SA</sub>@NC electrocatalysts feature nitrogen atoms coordinated to both Cu and Ru metal atoms via strong N-metal interactions. Density functional theory calculations revealed that alloyed CuRu nanoparticles and monodispersed Cu atoms are vital for altering the electronic configuration of the host Ru elements. This finely tuned structure enhanced the adsorption of H and OH and promoted CO oxidation over the N-(CuRu)<sub>NP+SA</sub>@NC electrocatalyst, resulting in high alkaline HOR activity, as evidenced by the higher exchange current density of 3.74 mA cm<sup>–2</sup> and high mass activity of 3.28 mA μg<sub>Ru</sub><sup>–1</sup>, which are far superior to those of most Ru-based catalysts reported to date. Moreover, the N-(CuRu)<sub>NP+SA</sub>@NC electrocatalysts are resistant to CO poisoning and can be used at a high concentration of 1000 ppm CO with no distinct decay in the activity, in stark contrast to the commercial Pt/C catalyst under the same conditions.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 266-276"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106188","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}

引用次数: 0

Structural dynamics of Ni/Mo2CTx MXene catalysts under reaction modulate CO2 reduction performance Ni/Mo2CTx MXene催化剂在反应调节CO2还原性能下的结构动力学

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-05-01 DOI: 10.1016/S1872-2067(25)64681-X

Jun Ma , Bing Xu , Shuo Cao , Shiyan Li , Wei Chu , Siglinda Perathoner , Gabriele Centi , Yuefeng Liu

{"title":"Structural dynamics of Ni/Mo2CTx MXene catalysts under reaction modulate CO2 reduction performance","authors":"Jun Ma , Bing Xu , Shuo Cao , Shiyan Li , Wei Chu , Siglinda Perathoner , Gabriele Centi , Yuefeng Liu","doi":"10.1016/S1872-2067(25)64681-X","DOIUrl":"10.1016/S1872-2067(25)64681-X","url":null,"abstract":"<div><div>The catalyst’s structural dynamics under reaction conditions critically determine their performance. We proved this indication by studying Ni nanoparticles supported on Mo<sub>2</sub>CT<sub><em>x</em></sub> MXene, where the average size during CO<sub>2</sub> hydrogenation changed from 12.9 to 3.1 nm. A parallel increase of CO selectivity from 21.1% to 92.6% at 400 °C was observed, while the CO<sub>2</sub> conversion rate remained at about 84.0 mmol·g<sub>cat</sub><sup>–1</sup>·h<sup>–1</sup>. This transformation involved partial removal of Mo<sub>2</sub>CT<sub><em>x</em></sub> terminal groups, allowing direct interaction between Ni and Mo atoms instead of indirect coupling through -O terminations. The shift from a Ni-O-Mo to a Ni-Mo interaction enhanced electron transfer from Ni to Mo<sub>2</sub>CT<sub><em>x</em></sub>, strengthening the metal-support interaction and driving Ni nanoparticle dispersion. <em>In-situ</em> mechanistic analysis and kinetic isotope studies revealed that Ni dispersion suppresses the formate and carboxyl pathway, promotes direct CO<sub>2</sub> dissociation, and inhibits CO hydrogenation, shifting the primary product from CH<sub>4</sub> to CO. These findings provide a strategy for designing highly selective and stable MXene-based catalysts through engineered metal-support interactions.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"72 ","pages":"Pages 243-253"},"PeriodicalIF":15.7,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106190","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}

引用次数: 0