Chinese Journal of Catalysis最新文献_第7页

Surface dynamics of Rh/Al2O3 during propane dehydrogenation 丙烷脱氢过程中 Rh/Al2O3 的表面动力学

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60063-X

Shuyi Li, Changle Mu, Nianqiu He, Jie Xu, Yanping Zheng, Mingshu Chen

{"title":"Surface dynamics of Rh/Al2O3 during propane dehydrogenation","authors":"Shuyi Li, Changle Mu, Nianqiu He, Jie Xu, Yanping Zheng, Mingshu Chen","doi":"10.1016/S1872-2067(24)60063-X","DOIUrl":"10.1016/S1872-2067(24)60063-X","url":null,"abstract":"<div>The surface structures of heterogeneous catalysts significantly impact catalytic performance, especially for structure-sensitive reactions. In this study, we employed surface techniques such as low-energy ion scattering spectroscopy, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy with CO as a probe (CO-FTIR) to investigate the surface dynamics of Rh/Al2O3 catalysts for propane dehydrogenation (PDH). We observed a notable induction process for PDH on Rh/Al2O3 catalysts, marked by significant variations in propane conversion, methane, and propylene selectivities. These changes were attributed to substantial coke formation. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy) and CO-FTIR revealed the coexistence of Rh nanoparticles, clusters, and single atoms on the surface. Through various dynamic quasi in-situ characterizations, we found that coke preferentially covered Rh clusters, thereby inhibiting C–C bond breaking and methane formation. Meanwhile, Rh single atoms were less affected by coke coverage and remained exposed as active and selective sites for PDH, favoring propylene production. This work underscores the sensitivity of PDH to the sizes of Rh species, with isolated Rh single atoms promoting propylene formation.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"62 ","pages":"Pages 145-155"},"PeriodicalIF":15.7,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141729189","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

Manipulating the interactions between N-intermediates and one-dimensional conjugated coordination polymers to boost electroreduction of nitrate to ammonia 操纵 N-中间体与一维共轭配位聚合物之间的相互作用，促进硝酸盐到氨的电还原反应

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60059-8

Qing Liu , Xue-Feng Cheng , Jin-Yan Huo , Xiao-Fang Liu , Huilong Dong , Hongbo Zeng , Qing-Feng Xu , Jian-Mei Lu

{"title":"Manipulating the interactions between N-intermediates and one-dimensional conjugated coordination polymers to boost electroreduction of nitrate to ammonia","authors":"Qing Liu , Xue-Feng Cheng , Jin-Yan Huo , Xiao-Fang Liu , Huilong Dong , Hongbo Zeng , Qing-Feng Xu , Jian-Mei Lu","doi":"10.1016/S1872-2067(24)60059-8","DOIUrl":"10.1016/S1872-2067(24)60059-8","url":null,"abstract":"<div>Electrocatalytic reduction of nitrate to ammonia (NITRR) is a promising strategy to remove nitrate pollutants and generate ammonia under mild conditions. However, the low conversion rate of nitrate and insufficient ammonia production rate severely limits the development of NITRR. Manipulating the adsorption of N-intermediates on the surface of catalyst greatly affects the activity and the selectivity of catalytic reaction. Herein, four one-dimensional π-d conjugated coordination polymers (1D CCPs) are synthesized and applied to NITRR. The selectivity and activity of NITRR are well improved by metal ion substitutions, which regulate the adsorption towards generated intermediates. The ammonia production rate reaches 2.28 mg h–1 cm–2 over Cu-BTA in 2 h, comparable to recent works at low nitrate concentrations, and the conversion rate of nitrate up to 96.74% in four hours with 79.46% ammonia selectivity. Density functional theory calculations reveal that Cu-BTA had electron-richer Cu center, causing the enhanced free energy of *NO and the attenuation of N=O bond. Therefore, the ΔG required for converting *NO to *NHO is reduced and the further hydrogenation is promoted. Additionally, the adsorption energies toward NH3 are also effectively reduced by metal ions substitution, accelerating the desorption of generated and adsorbed NH3, making the turnover of catalysts more frequent.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"62 ","pages":"Pages 231-242"},"PeriodicalIF":15.7,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141729658","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

Recent advances of the catalysts for photoelectrocatalytic oxygen evolution and CO2 reduction reactions 光电催化氧进化和二氧化碳还原反应催化剂的最新进展

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60053-7

Hong-Rui Zhu, Hui-Min Xu, Chen-Jin Huang, Zhi-Jie Zhang, Qi-Ni Zhan, Ting-Yu Shuai, Gao-Ren Li

{"title":"Recent advances of the catalysts for photoelectrocatalytic oxygen evolution and CO2 reduction reactions","authors":"Hong-Rui Zhu, Hui-Min Xu, Chen-Jin Huang, Zhi-Jie Zhang, Qi-Ni Zhan, Ting-Yu Shuai, Gao-Ren Li","doi":"10.1016/S1872-2067(24)60053-7","DOIUrl":"10.1016/S1872-2067(24)60053-7","url":null,"abstract":"<div>Increasing global energy consumption and environmental pollution make the use of new energy sources and environmentally friendly technologies essential to meet the diverse needs of industries. Photoelectrocatalysis is a promising method of utilising solar and electrical energy for various catalytic reactions with significant environmental and energy saving benefits. And photoelectrocatalytic (PEC) oxygen evolution reaction (OER) and CO2 reduction reaction (CO2RR) are two catalytic reactions with great potential for energy and environmental applications. PEC OER is critical for renewable energy technologies for water oxidation and other related oxidation reactions. PEC CO2RR converts carbon dioxide into high-value products via a catalyst, enabling the rational use of carbon dioxide and the reduction of greenhouse gas emissions. Both technologies are efficient, environmentally friendly, and sustainable. However, further research and optimisation are needed to promote the industrial application of both technologies for energy conversion and environmental protection. This paper reviews the research progress of PEC CO2RR and OER catalysts in recent years, including detailed descriptions of catalyst types, reaction mechanisms and performance tests. Finally, the paper considers the future trends and prospects of PEC technology, providing new insights into the technology and research directions for PEC OER and CO2RR catalysts.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"62 ","pages":"Pages 53-107"},"PeriodicalIF":15.7,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141729185","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

Coordination dynamics of iron enables the selective C–N coupling but bypasses unwanted C–H hydroxylation in Fe(II)/α-ketoglutarate- dependent non-heme enzymes 铁的配位动力学使铁(II)/α-酮戊二酸依赖性非血红素酶中的选择性 C-N 偶联得以实现，但绕过了不需要的 C-H 羟基化反应

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60064-1

Xuan Zhang , Jia Liu , Langxing Liao , Zikuan Wang , Binju Wang

{"title":"Coordination dynamics of iron enables the selective C–N coupling but bypasses unwanted C–H hydroxylation in Fe(II)/α-ketoglutarate- dependent non-heme enzymes","authors":"Xuan Zhang , Jia Liu , Langxing Liao , Zikuan Wang , Binju Wang","doi":"10.1016/S1872-2067(24)60064-1","DOIUrl":"10.1016/S1872-2067(24)60064-1","url":null,"abstract":"<div>Non-heme Fe(II)/α-ketoglutarate (αKG)-dependent enzymes catalyze numerous C–H activation and functionalization reactions. However, how αKG-dependent non-heme enzymes catalyzed C–H functionalization beyond the hydroxylation is largely unknown. Here, we addressed this issue in Fe(II)/ αKG-dependent oxygenase TqaLNc, which catalyzes the selective C–H amination but bypasses the thermodynamically favored C–H hydroxylation. Here, the extensive computational studies have shown that the aziridine formation involves the conformational change of the Fe(IV)=O species from the axial configuration to the equatorial one, the substrate deprotonation of NH3+ group to form the NH-ligated intermediate, the C–H activation by the equatorial Fe(IV)=O species. Such mechanistic scenario has been cross-validated by oxidation of various substrates by TqaLNc and its variants, including the available experiments and our new experiments. While the presence of steric hindrance between the substrate and the second-sphere residues would inhibit the aziridination process, the intrinsic reactivity of aziridination vs. hydroxylation is dictated by the energy splitting between two key redox-active dπ* frontier molecular orbitals: dπ*Fe-N and dπ*Fe-OH. The present findings highlight the key roles of the coordination change and dynamics of iron cofactor in dictating the catalysis of non-heme enzymes and have far-reaching implications for the other non-heme Fe(II)/αKG-dependent enzymes catalyzed C–H functionalization beyond the hydroxylation.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"62 ","pages":"Pages 131-144"},"PeriodicalIF":15.7,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141729188","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

Proton feeding from defect-rich carbon support to cobalt phthalocyanine for efficient CO2 electroreduction 从富含缺陷的碳支持物向酞菁钴提供质子，实现高效的二氧化碳电还原

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60061-6

Ziwen Mei, Kejun Chen, Yao Tan, Qiuwen Liu, Qin Chen, Qiyou Wang, Xiqing Wang, Chao Cai, Kang Liu, Junwei Fu, Min Liu

{"title":"Proton feeding from defect-rich carbon support to cobalt phthalocyanine for efficient CO2 electroreduction","authors":"Ziwen Mei, Kejun Chen, Yao Tan, Qiuwen Liu, Qin Chen, Qiyou Wang, Xiqing Wang, Chao Cai, Kang Liu, Junwei Fu, Min Liu","doi":"10.1016/S1872-2067(24)60061-6","DOIUrl":"10.1016/S1872-2067(24)60061-6","url":null,"abstract":"<div>Electrocatalytic CO2 reduction reaction (CO2RR) holds significant promise for sustainable energy conversion, with cobalt phthalocyanine (CoPc) emerging as a notable catalyst due to its high CO selectivity. However, CoPc's efficacy is hindered by its limited ability to provide sufficient proton for the protonation process, particularly at industrial current densities. Herein, we introduce defect-engineered carbon nanotubes (d-CNT) to augment proton feeding for CO2RR over CoPc, achieved by expediting water dissociation. Our kinetic measurements and in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy reveal d-CNT significantly enhances proton feeding, thereby facilitating CO2 activation to *COOH in CoPc. Density functional theory calculations corroborate these findings, illustrating that d-CNT decreases the barrier to water dissociation. Consequently, the CoPc/d-CNT mixture demonstrates robust performance, achieving 500 mA cm–2 for CO2RR with CO selectivity exceeding 96%. Notably, CoPc/d-CNT remains stability for a duration of 20 h under a substantial current density of 150 mA cm–2. The study broadens the scope of practical applications for molecular catalysts in CO2RR, marking a significant step towards sustainable energy conversion.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"62 ","pages":"Pages 190-197"},"PeriodicalIF":15.7,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141729217","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

Rational design of Pt-anchored single-atom alloy electrocatalysts for NO-to-NH3 conversion by density functional theory and machine learning 通过密度泛函理论和机器学习合理设计用于 NO-NH3 转化的铂锚定单原子合金电催化剂

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60078-1

Jieyu Liu , Haiqiang Guo , Yulin Xiong , Xing Chen , Yifu Yu , Changhong Wang

{"title":"Rational design of Pt-anchored single-atom alloy electrocatalysts for NO-to-NH3 conversion by density functional theory and machine learning","authors":"Jieyu Liu , Haiqiang Guo , Yulin Xiong , Xing Chen , Yifu Yu , Changhong Wang","doi":"10.1016/S1872-2067(24)60078-1","DOIUrl":"10.1016/S1872-2067(24)60078-1","url":null,"abstract":"<div>Electrochemical NO reduction reaction (NORR) toward NH3 synthesis emerges as a promising approach to eliminate NO pollution and generate high-value-added products simultaneously. Therefore, exploring suitable NORR electrocatalysts is of great importance. Here, we present a design principle to evaluate the activity of single-atom alloy catalysts (SAACs), whose excellent catalytic performance and well-defined bonding environments make them suitable candidates for studying structure-activity relationships. The machine learning (ML) algorithm is chosen to unveil the underlying physics and chemistry. The results indicate that the catalytic activity of SAACs is highly correlated with the local environment of the active center, that is, the atomic and electronic features. The coeffect of these features is quantitatively verified by adopting a data-driven method. The combination of density functional theory (DFT) and ML investigations not only provides an understanding of the complex NORR mechanisms but also offers a strategy to design highly efficient SAACs with specific active centers rationally.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"62 ","pages":"Pages 243-253"},"PeriodicalIF":15.7,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141729638","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

An efficient and stable high-entropy alloy electrocatalyst for hydrogen evolution reaction 用于氢气进化反应的高效稳定的高熵合金电催化剂

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60067-7

Gui Zhao , Kuan Lu , Yunan Li , Fagui Lu , Peng Gao , Bing Nan , Lina Li , Yixiao Zhang , Pengtao Xu , Xi Liu , Liwei Chen

{"title":"An efficient and stable high-entropy alloy electrocatalyst for hydrogen evolution reaction","authors":"Gui Zhao , Kuan Lu , Yunan Li , Fagui Lu , Peng Gao , Bing Nan , Lina Li , Yixiao Zhang , Pengtao Xu , Xi Liu , Liwei Chen","doi":"10.1016/S1872-2067(24)60067-7","DOIUrl":"10.1016/S1872-2067(24)60067-7","url":null,"abstract":"<div>High-entropy alloy (HEA) catalysts exhibit enhanced hydrogen evolution reaction (HER) activity in water electrolysis, yet the understanding of their structure and active sites in reaction environments remains unclear. Here, we systematically investigated the HER activity and stability of PtPdRhRuCu/C through a combination of electrochemical measurements, in situ synchrotron radiation X-ray absorption spectroscopy (XAS) at the Cu K-edge and Pt L3-edge, and density functional theory (DFT) calculations. Uniformly sized PtPdRhRuCu HEA nanoparticles were prepared via a facile one-step solvothermal method. In situ XAS results revealed that the HEA nanoparticles maintained metallic states and a disordered arrangement of the overall structure at hydrogen evolution potential, implying the absence of the separated phases. Relying on multi-metal active sites, PtPdRhRuCu/C demonstrated a remarkably low overpotential of 23.3 mV at 10 mA cm–2 in alkaline HER, which is significantly lower than the overpotential observed in commercial Pt/C (50.3 mV), and achieving a mass activity 7.9 times that of Pt/C. DFT calculations show that the synergy of each metal site optimizes the dissociation energy barrier of water molecules. This study not only demonstrates the advancement of high-entropy alloys in electrocatalysis but also provides a comprehensive understanding of the structure-activity relationship of these unique catalysts through detailed characterizations. Our findings further contribute to the rational design and application of high-entropy alloy catalysts, specifically in HER.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"62 ","pages":"Pages 156-165"},"PeriodicalIF":15.7,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141729190","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

Large-current polarization-engineered FeOOH@NiOOH electrocatalyst with stable Fe sites for large-current oxygen evolution reaction 具有稳定铁位点的大电流极化工程化 FeOOH@NiOOH 电催化剂用于大电流氧进化反应

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60062-8

Qingyun Lv , Weiwei Zhang , Zhipeng Long , Jiantao Wang , Xingli Zou , Wei Ren , Long Hou , Xionggang Lu , Yufeng Zhao , Xing Yu , Xi Li

{"title":"Large-current polarization-engineered FeOOH@NiOOH electrocatalyst with stable Fe sites for large-current oxygen evolution reaction","authors":"Qingyun Lv , Weiwei Zhang , Zhipeng Long , Jiantao Wang , Xingli Zou , Wei Ren , Long Hou , Xionggang Lu , Yufeng Zhao , Xing Yu , Xi Li","doi":"10.1016/S1872-2067(24)60062-8","DOIUrl":"10.1016/S1872-2067(24)60062-8","url":null,"abstract":"<div>NiFe-based (oxy)hydroxides are among the most efficient electrocatalysts for the oxygen evolution reaction (OER). However, significant Fe leakage during the OER results in unsatisfactory stability. Herein, a large-current (1.5 A cm–2) galvanostatic reconstruction was used to fabricate FeOOH@NiOOH (eFNOL) with both fixed Fe sites and exposed high-index crystal facets (HIFs). Compared to FeNiOOH with low-index crystal facets, the phase-separated FeOOH@NiOOH showed a higher binding energy towards Fe, and the HIFs significantly improved the catalytic activity of FeOOH. The optimized eFNOL catalyst exhibits ultralow overpotentials of 234 and 272 mV, yielding substantial current densities of 100 and 500 mA cm–2, respectively, with a small Tafel slope of 35.2 mV dec–1. Moreover, due to the stabilized Fe sites, its striking stability over 100 h at 500 mA cm–2 with 1.5% decay outperforms most NiFe-based OER catalysts reported recently. This study provides an effective strategy for developing highly active and stable catalysts via large-current electrochemical reconstruction.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"62 ","pages":"Pages 254-264"},"PeriodicalIF":15.7,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141729639","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

Synergistic photoelectric and thermal effect for efficient nitrate reduction on plasmonic Cu photocathodes 等离子铜光电阴极上高效硝酸盐还原的光电和热协同效应

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60060-4

Zhenlin Chen , Jing Xue , Lei Wu , Kun Dang , Hongwei Ji , Chuncheng Chen , Yuchao Zhang , Jincai Zhao

{"title":"Synergistic photoelectric and thermal effect for efficient nitrate reduction on plasmonic Cu photocathodes","authors":"Zhenlin Chen , Jing Xue , Lei Wu , Kun Dang , Hongwei Ji , Chuncheng Chen , Yuchao Zhang , Jincai Zhao","doi":"10.1016/S1872-2067(24)60060-4","DOIUrl":"10.1016/S1872-2067(24)60060-4","url":null,"abstract":"<div>Recently, electrochemical nitrate reduction reaction (NO3RR) has been intensively explored for the synthesis of ammonia, and copper (Cu) has become one of the most promising materials for NO3RR. Notably, Cu is an important plasmonic metal that absorbs visible light. The plasmonic effect might have a significant influence on the performance of Cu-catalyzed NO3RR but has been seldom reported. Herein, we report the synergistic photoelectric and thermal effect for efficient and stable NO3RR on plasmonic Cu nanowire photocathodes, which is exclusively effective for NO3RR but has no effect on the competing hydrogen evolution reaction. The faradaic efficiency for ammonia production is nearly 100% within a potential range from –0.2 V to –0.4 V vs. RHE, and a high ammonia yield rate of 1.37 mmol h–1 cm–2 is achieved at –0.2 V vs. RHE. Further operando photoelectrochemical studies and theoretical simulations confirm that the plasmonic excitation efficiently accelerates the rate-limiting desorption of NH3 on Cu surfaces. We further demonstrate the versatility of this strategy to other Cu-based nanostructures.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"62 ","pages":"Pages 219-230"},"PeriodicalIF":15.7,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141729657","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

Asymmetric oxygen vacancies in La2FeMO6 double perovskite for boosting oxygen activation and H2S selective oxidation 促进氧活化和 H2S 选择性氧化的 La2FeMO6 双包晶石中的不对称氧空位

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60051-3

Zheng Wei, Guoxia Jiang, Yiwen Wang, Ganggang Li, Zhongshen Zhang, Jie Cheng, Fenglian Zhang, Zhengping Hao

{"title":"Asymmetric oxygen vacancies in La2FeMO6 double perovskite for boosting oxygen activation and H2S selective oxidation","authors":"Zheng Wei, Guoxia Jiang, Yiwen Wang, Ganggang Li, Zhongshen Zhang, Jie Cheng, Fenglian Zhang, Zhengping Hao","doi":"10.1016/S1872-2067(24)60051-3","DOIUrl":"10.1016/S1872-2067(24)60051-3","url":null,"abstract":"<div>Tuning oxygen vacancy (VO) in metal oxides catalysts that efficiently activates O2 molecule to promote oxidation reactions remains challenging. Herein, transition metal (M = Mn, Co, and Mo) doping was used to moderate the coordination environment of VO in La2FeMO6 and promote activity for selective oxidation of hydrogen sulfide (H2S). Various techniques reveal that the introduction of Mn and Co forms the homogeneous double perovskite phase, which results in the formation of asymmetric VO. Although these asymmetric VO are more difficult to form than symmetric Fe-VO-Fe due to the shorter bond distance and stronger bond strength of Fe-O, they are more conducive to the dissociation of O2 molecules. Among them, the formed rich Fe-VO-Mn sites from the alternate substitution of Mn to Fe boosted the activation of O2 molecules of Mn-substituted LaFeO3. Therefore, enhanced catalytic activity and outstanding sulfur selectivity were achieved as a result of promoted oxygen mobility and reducibility. This work provides an attractive strategy for rational design of advanced oxidation catalysts.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"62 ","pages":"Pages 198-208"},"PeriodicalIF":15.7,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141729655","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