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Coupling of BiOCl Ultrathin Nanosheets with Carbon Quantum Dots for Enhanced Photocatalytic Performance
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作者 Pin Song Xiaoyu Fang +14 位作者 Wei Jiang Yuyang Cao Daobin Liu Shiqiang Wei Jun Du Lang Sun Lei Zhao Song Liu Yuzhu Zhou Jun Di Chade Lv Bijun Tang Jiefu Yang Tingting Kong yujie xiong 《Transactions of Tianjin University》 EI CAS 2024年第3期211-220,共10页
Over the past few decades,photocatalysis technology has received extensive attention because of its potential to mitigate or solve energy and environmental pollution problems.Designing novel materials with outstanding... Over the past few decades,photocatalysis technology has received extensive attention because of its potential to mitigate or solve energy and environmental pollution problems.Designing novel materials with outstanding photocatalytic activities has become a research hotspot in this field.In this study,we prepared a series of photocatalysts in which BiOCl nanosheets were modified with carbon quantum dots(CQDs)to form CQDs/BiOCl composites by using a simple solvothermal method.The photocatalytic performance of the resulting CQDs/BiOCl composite photocatalysts was assessed by rhodamine B and tetracycline degradation under visible-light irradiation.Compared with bare BiOCl,the photocatalytic activity of the CQDs/BiOCl composites was significantly enhanced,and the 5 wt%CQDs/BiOCl composite exhibited the highest photocatalytic activity with a degradation efficiency of 94.5%after 30 min of irradiation.Moreover,photocatalytic N_(2)reduction performance was significantly improved after introducing CQDs.The 5 wt%CQDs/BiOCl composite displayed the highest photocatalytic N_(2)reduction performance to yield NH_3(346.25μmol/(g h)),which is significantly higher than those of 3 wt%CQDs/BiOCl(256.04μmol/(g h)),7 wt%CQDs/BiOCl(254.07μmol/(g h)),and bare BiOCl(240.19μmol/(g h)).Our systematic characterizations revealed that the key role of CQDs in improving photocatalytic performance is due to their increased light harvesting capacity,remarkable electron transfer ability,and higher photocatalytic activity sites. 展开更多
关键词 Carbon quantum dots BiOCl Rhodamine B TETRACYCLINE PHOTOCATALYSIS
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Defect engineering: A versatile tool for tuning the activation of key molecules in photocatalytic reactions 被引量:9
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作者 Ning Zhang Chao Gao yujie xiong 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2019年第10期43-57,共15页
Many photocatalytic reactions such as CO2 reduction and N2 fixation are often limited by the activation of some key molecules. Defects in solid materials can robustly introduce coordinately unsaturated sites to serve ... Many photocatalytic reactions such as CO2 reduction and N2 fixation are often limited by the activation of some key molecules. Defects in solid materials can robustly introduce coordinately unsaturated sites to serve as highly active sites for molecular chemisorption and activation. As a result, rational defect engineering has endowed a versatile approach to further develop photocatalytic applications beyond water splitting. The subtly designed defects in photocatalysts can play critical and decisive roles in molecular activation as proven in recent years. The defects cannot only serve as active sites for molecular chemisorption, but also spatially supply channels for energy and electron transfer. In this review, we aim to summarize the diversiform photocatalytic applications using defects as active sites, including but not limited to CO2 reduction, O2 activation,H2O dissociation, N2 fixation as well as activation of other molecules. In particular, we emphatically outline how the parameters of defects (e.g.,concentration,location,geometric and electronic structures) can serve as the knobs for maneuvering molecular adsorption and activation as well as altering subsequent reaction pathway. Moreover, we underline the remaining challenges at the current stage and the potential development in the future.It is anticipated that this review consolidates the in-depth understanding towards the structure-activity relationship between defects and related reactions. 展开更多
关键词 DEFECT engineering PHOTOCATALYSIS MOLECULAR adsorption MOLECULAR activation Electron transfer
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Tuning the local coordination environment of silver(Ⅰ) coordination networks with counterions for enhanced electrocatalytic CO_(2) reduction
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作者 Xiaofeng Cui Xueting Wang +4 位作者 Cong Fu Bing Liu Mei-Yan Gao Tingting Kong yujie xiong 《Science China Chemistry》 SCIE EI CAS CSCD 2024年第5期1524-1530,共7页
Very recently, the local coordination environment of active sites has been found to strongly influence their performance in electrocatalytic CO_(2) reduction by tuning the intrinsic kinetics of CO_(2) activation and i... Very recently, the local coordination environment of active sites has been found to strongly influence their performance in electrocatalytic CO_(2) reduction by tuning the intrinsic kinetics of CO_(2) activation and intermediate stabilization. It is imperative to elucidate the mechanism for such an influence towards the rational design of efficient catalysts;however, the complex interactions between the multiple factors involved in the system make it challenging to establish a clear structure–performance relationship. In this work, we chose ion-intercalated silver(I)-based coordination networks(AgCNs) with a well-defined structure as a model platform, which enables us to understand the regulation mechanism of counterions as the counterions are the only tuning factor involved in such a system. We prepared two isostructural Ag CNs with different intercalation ions or counterions of BF_(4)^(-) and ClO_(4)^(-)(named as AgCNs-BF_(4) and AgCNs-ClO_(4)) and found that the former has a more competitive CO_(2) electroreduction performance than the latter. AgCNs-BF_(4) achieves the highest Faradaic efficiency for CO_(2) to CO of 87.1% at-1.0 V(vs. RHE) with a higher partial current density, while AgCNs-ClO_(4) exhibits only 77.2% at the same applied potential.Spectroscopic characterizations and theoretical calculation reveal that the presence of BF_(4)^(-)is more favorable for stabilizing the COOH^(*) intermediate by weakening hydrogen bonds, which accounts for the superior activity of Ag CNs-BF_(4). 展开更多
关键词 electrocatalytic CO_(2) reduction coordination networks local environment COUNTERIONS intercalation ions
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Bridging molecular photosensitizer and catalyst on carbon nanotubes toward enhanced selectivity and durability for CO_(2)photoreduction
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作者 Xiaofeng Cui Xueting Wang +3 位作者 Lijun Zhao Jixin Wang Tingting Kong yujie xiong 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2024年第6期157-164,共8页
Homogenous molecular photocatalysts for CO_(2)reduction,especially metal complex-based photosensitizer-catalyst assemblages,have been attracting extensive research interests due to their efficiency and customizability... Homogenous molecular photocatalysts for CO_(2)reduction,especially metal complex-based photosensitizer-catalyst assemblages,have been attracting extensive research interests due to their efficiency and customizability.However,their low durability and recyclability limit practical applications.In this work,we immobilized the catalysts of metal terpyridyl complexes and the photosensitizer of[Ru(bpy)3]Cl2onto the surface of carbon nanotubes through covalent bonds and electrostatic interactions,respectively,transforming the homogeneous system into a heterogeneous one.Our characterizations prove that these metal complexes are well dispersed on CNTs with a high loading(ca.12 wt.%).Photocatalytic measurements reveal that catalytic activity is remarkably enhanced when the molecular catalysts are anchored,which is three times higher than that of homogeneous molecular catalysts.Moreover,when the photosensitizer of[Ru(bpy)3]Cl2is immobilized,the side reaction of hydrogen evolution is completely suppressed and the selectivity for CO production reaches 100%,with its durability also significantly improved.This work provides an effective pathway for constructing heterogeneous photocatalysts based on rational assembly of efficient molecular photosensitizers and catalysts. 展开更多
关键词 DURABILITY SELECTIVITY CATALYST
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Integration of Green Hydrogen Production and Storage via Electrocatalysis
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作者 Chao Zhang Jingxiang Low yujie xiong 《Precision Chemistry》 2024年第6期229-238,共10页
Hydrogen economy,which proposes employing hydrogen to replace or supplement the current fossil-fuel-based energy economy system,is widely accepted as the future energy scheme for the sustainable and green development ... Hydrogen economy,which proposes employing hydrogen to replace or supplement the current fossil-fuel-based energy economy system,is widely accepted as the future energy scheme for the sustainable and green development of human society.While the hydrogen economy has shown tremendous potential,the associated challenges with hydrogen production and storage remain significant barriers to wide applications.In light of this consideration,the integration of green hydrogen production and storage through electrocatalysis for direct production of chemical hydrogen storage media has emerged as a potential solution to these challenges.Specifically,through electrocatalysis,CO_(2) and H_(2)O can be converted into methanol or formic acid,while N_(2) or NOx along with H_(2)O can be transformed into ammonia,streamlining the hydrogen economy scheme.In this Perspective,we provide an overview of recent developments in this technology.Additionally,we briefly discuss the general properties and corresponding production strategies via the electrolysis of these chemical hydrogen storage media.Finally,we conclude by offering insights into future perspectives in this field,anticipating that the successful advancement of such technology will propel the development of the hydrogen economy toward practical implementation. 展开更多
关键词 Hydrogen economy ELECTROCATALYSIS METHANOL Formic acid AMMONIA
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Cu_(2−x)S derived copper nanoparticles:A platform for unraveling the role of surface reconstruction in efficient electrocatalytic CO_(2)-to-C_(2)H_(4)conversion 被引量:3
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作者 Chaohua He Delong Duan +7 位作者 Jingxiang Low Yu Bai Yawen Jiang Xinyu Wang Shuangming Chen Ran Long Li Song yujie xiong 《Nano Research》 SCIE EI CSCD 2023年第4期4494-4498,共5页
Cu-based electrocatalysts have provoked much attention for their high activity and selectivity in carbon dioxide(CO_(2))conversion into multi-carbon hydrocarbons.However,during the electrochemical reaction,Cu catalyst... Cu-based electrocatalysts have provoked much attention for their high activity and selectivity in carbon dioxide(CO_(2))conversion into multi-carbon hydrocarbons.However,during the electrochemical reaction,Cu catalysts inevitably undergo surface reconstruction whose impact on CO_(2)conversion performance remains contentious.Here we report that polycrystalline Cu nanoparticles(denoted as Cu-s)with rich high-index facets,derived from Cu_(2−x)S through desulphurization and surface reconstruction,offer an excellent platform for investigating the role of surface reconstruction in electrocatalytic CO_(2)conversion.During the formation of Cu-s catalyst,the two stages of desulphurization and surface reconstruction can be clearly resolved by in situ X-ray absorption spectroscopy and OH−adsorption characterizations,which are well correlated with the changes in electrocatalytic performance.It turns out that the high CO_(2)conversion performance,achieved by the Cu-s catalyst(Faradic efficiency of 68.6%and partial current density of 40.8 mA/cm^(2)in H-cell toward C_(2)H_(4)production),is attributed to the increased percentage of high-index facets in Cu-s during the surface reconstruction.Furthermore,the operando electrochemical Raman spectroscopy further reveals that the conversion of the CO_(2)into the C_(2)H_(4)on Cu-s is intermediated by the production of*COCHO.Our findings manifest that the surface reconstruction is an effective method for tuning the reaction intermediate of the CO_(2)conversion toward high-value multicarbon(C2+)chemicals,and highlight the significance of in situ characterizations in enhancing the understanding of the surface structure and its role in electrocatalysis. 展开更多
关键词 CO_(2)electroreduction reaction surface reconstruction high-index facets ethylene(C_(2)H_(4)) Cu catalysts
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Biomass-derived hard carbon microtubes with tunable apertures for high-performance sodium-ion batteries 被引量:3
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作者 Pin Song Shiqiang Wei +12 位作者 Jun Di Jun Du Wenjie Xu Daobin Liu Changda Wang Sicong Qiao Yuyang Cao Qilong Cui Pengjun Zhang Liaobo Ma Jiewu Cui Yan Wang yujie xiong 《Nano Research》 SCIE EI CSCD 2023年第4期4874-4879,共6页
Sodium-ion batteries(SIBs)are considered the most up-and-coming complements for large-scale energy storage devices due to the abundance and cheap sodium.However,due to the bigger radius,it is still a great challenge t... Sodium-ion batteries(SIBs)are considered the most up-and-coming complements for large-scale energy storage devices due to the abundance and cheap sodium.However,due to the bigger radius,it is still a great challenge to develop anode materials with suitable space for the intercalation of sodium ions.Herein,we present hard carbon microtubes(HCTs)with tunable apertures derived from low-cost natural kapok fibers via a carbonization process for SIBs.The resulted HCTs feature with smaller surface area and shorter Na+diffusion path benefitting from their unique micro-nano structure.Most importantly,the wall thickness of HCTs could be regulated and controlled by the carbonization temperature.At a high temperature of 1,600℃,the carbonized HCTs possess the smallest wall thickness,which reduces the diffusion barrier of Na+and enhances the reversibility Na+storage.As a result,the 1600HCTs deliver a high initial Coulombic efficiency of 90%,good cycling stability(89.4%of capacity retention over 100 cycles at 100 mA·g^(−1)),and excellent rate capacity.This work not only charts a new path for preparing hard carbon materials with adequate ion channels and novel tubular micro-nano structures but also unravels the mechanism of hard carbon materials for sodium storage. 展开更多
关键词 hard carbon kapok fibers sodium-ion batteries(SIBs) reversible capacity long cycle life
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Biosynthetic CdS-Thiobacillus thioparus hybrid for solar-driven carbon dioxide fixation 被引量:2
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作者 Guangyu Liu Feng Gao +3 位作者 Hongwei Zhang Lei Wang Chao Gao yujie xiong 《Nano Research》 SCIE EI CSCD 2023年第4期4531-4538,共8页
Synergistically combining biological whole-cell bacteria with man-made semiconductor materials innovates the way for sustainable solar-driven CO_(2)fixation,showing great promise to break through the bottleneck in tra... Synergistically combining biological whole-cell bacteria with man-made semiconductor materials innovates the way for sustainable solar-driven CO_(2)fixation,showing great promise to break through the bottleneck in traditional chemical photocatalyst systems.However,most of the biohybrids require uneconomical organic nutrients and anaerobic conditions for the successful cultivation of the bacteria to sustain the CO_(2)fixation,which severely limits their economic viability and applicability for practical application.Herein,we present an inorganic-biological hybrid system composed of obligate autotrophic bacteria Thiobacillus thioparus(T.thioparus)and CdS nanoparticles(NPs)biologically precipitated on the bacterial surface,which can achieve efficient CO_(2)fixation based entirely on cost-effective inorganic salts and without the restriction of anaerobic conditions.The optimized interface between CdS NPs and T.thioparus formed by biological precipitation plays an essential role for T.thioparus efficiently receiving photogenerated electrons from CdS NPs and thus changing the autotrophic way from chemoautotroph to photoautotroph.As a result,the CdS-T.thioparus biohybrid realizes the solar-driven CO_(2)fixation to produce multi-carbon glutamate synthase and biomass under visible-light irradiation with CO_(2)as the only carbon source.This work provides significant inspiration for the further exploration of the solar-driven self-replicating biocatalytic system to achieve CO_(2)fixation and conversion. 展开更多
关键词 biohybrids solar-driven CO_(2)fixation carbon cycle autotrophic bacteria Thiobacillus thioparus cadmium sulfide
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Recent progress in electrochemical C–N coupling reactions 被引量:3
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作者 Yuan Zhong Hailong xiong +2 位作者 Jingxiang Low Ran Long yujie xiong 《eScience》 2023年第1期26-37,共12页
Electrochemical C–N coupling has generated intense research interest as a promising approach to reduce carbon and nitrogen emissions and store excess renewable electricity in valuable chemicals(e.g.,urea,amides,and a... Electrochemical C–N coupling has generated intense research interest as a promising approach to reduce carbon and nitrogen emissions and store excess renewable electricity in valuable chemicals(e.g.,urea,amides,and amines).In this review,we discuss the emerging trends in electrocatalytic C–N coupling reactions using CO_(2) and inorganic nitrogenous species(i.e.,dinitrogen(N_(2))),nitrate(NO_(2)^(-)),nitrite(NO_(3)^(-)),and ammonia(NH_(3))as raw materials.The related reaction mechanisms and potential design principles for advanced electrocatalysts are outlined.In addition,the effects of different reactors,including H-cells,membrane-based flow reactors,and membrane electrode assembly electrolyzers,on the coupling reactions are emphasized.Finally,the current challenges and future opportunities in this field are described.We aim to provide an up-to-date overview of the electrochemical C–N coupling system to advance progress toward its practical application. 展开更多
关键词 Electrochemical C-N coupling reactions Carbon dioxide Inorganic nitrogenous species Nitrogenous compounds Reactor designs
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Engineering active Ni-doped Co_(2)P catalyst for efficient electrooxidation coupled with hydrogen evolution 被引量:1
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作者 Jiayi Li Xin Mao +5 位作者 Wanbing Gong Xinyu Wang Yawen Jiang Ran Long Aijun Du yujie xiong 《Nano Research》 SCIE EI CSCD 2023年第5期6728-6735,共8页
The thermodynamically favorable electrocatalytic oxidation coupled with hydrogen evolution reaction(HER)is considered as a sustainable and promising technique.Nonetheless,it remains a great challenge due to the lack o... The thermodynamically favorable electrocatalytic oxidation coupled with hydrogen evolution reaction(HER)is considered as a sustainable and promising technique.Nonetheless,it remains a great challenge due to the lack of simple,cheap,highefficient electrocatalysts.Here,we successfully develop a simple and scalable electro-deposition and subsequent phosphorization route to fabricate Ni-doped Co_(2)P(Ni-Co_(2)P)nanosheets catalyst using the in-situ released Ni species from defective Ni foam as metal source.Impressively,the as-synthesized Ni-Co_(2)P catalyst exhibits excellent electrochemical 5-hydroxymethylfurfural oxidation reaction(HOR)performance with>99%2,5-furandicarboxylic acid yield and>97%Faradaic efficiency at an ultralow potential of 1.29 V vs.reversible hydrogen electrode(RHE).Experimental characterization and theoretical calculation reveal that the atomically doped Ni species can enhance the adsorption of reactant and thus lower the reaction energy barriers.By coupling the electrocatalytic HOR with HER,the employed two-electrode system using Ni-Co_(2)P and commercial Ni foam as anode and cathode,respectively,exhibits a low cell voltage of 1.53 V to drive a current density of 10 mA·cm^(−2),which is 90 mV lower than that of pure water splitting.This work provides a facile and efficient approach for the preparation of high-performance earth-abundant electrocatalysts toward the concurrent production of H_(2)and value-added chemicals. 展开更多
关键词 heteroatomic doping phosphide electrodes electrocatalytic oxidation hydrogen evolution reaction biomass conversion
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Boosting electrochemical hydrogen evolution by coupling anodically oxidative dehydrogenation of benzylamine to benzonitrile 被引量:1
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作者 Kun Chen Wei Zhang +4 位作者 Yu Bai Wanbing Gong Ning Zhang Ran Long yujie xiong 《Chinese Chemical Letters》 SCIE CAS CSCD 2023年第3期460-464,共5页
The electricity-driven water splitting acts as a promising pathway for renewable energy conversion and storage, yet anodic oxygen evolution reaction(OER) largely hinders its efficiency. Seeking the alternatives to OER... The electricity-driven water splitting acts as a promising pathway for renewable energy conversion and storage, yet anodic oxygen evolution reaction(OER) largely hinders its efficiency. Seeking the alternatives to OER exhibits the competitive advance to address this predicament. In this work, we show a more thermodynamically and kinetically favorable reaction, electrochemical oxidative dehydrogenation(EODH)of benzylamine to replace the conventional OER, catalyzed by a cobalt cyclotetraphosphate(Co_(2)P_(4)O_(12)) nanorods catalyst grown on nickel foam. This anodic reaction lowers the electricity input of 317 mV toward the desired current density of 100 mA/cm^(2), together with a highly selective benzonitrile product of more than 97%. More specifically, when coupling it with cathodic hydrogen evolution reaction(HER),the proposed HER||benzylamine-EODH configuration only requires a cell voltage of 1.47 V@100 mA/cm^(2),exhibiting an energy-saving up to 17% relative to conventional water splitting, as well as the near unit selectivity toward cathodic H_(2) and anodic benzonitrile products. 展开更多
关键词 ELECTROSYNTHESIS Benzylamine dehydrogenation COUPLING Hydrogen evolution Cobalt cyclotetraphosphate
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Highly Efficient and Selective Photocatalytic Nonoxidative Coupling of Methane to Ethylene over Pd-Zn Synergistic Catalytic Sites
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作者 Yanduo Liu Yihong Chen +4 位作者 Wenbin Jiang Tingting Kong Pedro H.C.Camargo Chao Gao yujie xiong 《Research》 EI CAS CSCD 2023年第1期485-496,共12页
Photocatalytic nonoxidative coupling of CH_(4)to multicarbon(C^(2+))hydrocarbons(e.g.,C,H4)and H,under ambient conditions provides a promising energy-conserving approach for utilization of carbon resource.However,as t... Photocatalytic nonoxidative coupling of CH_(4)to multicarbon(C^(2+))hydrocarbons(e.g.,C,H4)and H,under ambient conditions provides a promising energy-conserving approach for utilization of carbon resource.However,as the methyl intermediates prefer to undergo self-coupling to produce ethane,it is a challenging task to control the selective conversion of CH to higher valueadded CH4.Herein,we adopt a synergistic catalysis strategy by integrating Pd-Zn active sites on visible light-responsive defective WO_(3)nanosheets for synergizing the adsorption,activation,and dehydrogenation processes in CH_(4)to C_(2)H_(4)conversion.Benefiting from the synergy,our model catalyst achieves a remarkable C^(2+)compounds yield of 31.85μmolgh with an exceptionally high C,H4 selectivity of 75.3%and a stoichiometric H_(2)evolution.In situ spectroscopic studies reveal that the Zn sites promote the adsorption and activation of CH_(4)molecules to generate methyl and methoxy intermediates with the assistance of lattice oxygen,while the Pd sites facilitate the dehydrogenation of methoxy to methylene radicals for producing C_(2)H_(4)and suppress overoxidation.This work demonstrates a strategy for designing efficient photocatalysts toward selective coupling of CH_(4)to higher value-added chemicals and highlights the importance of synergistic active sites to the synergy of key steps in catalytic reactions. 展开更多
关键词 OXIDATIVE SYNERGISTIC coupling
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胺功能化的铜催化剂:氢键介导的电化学CO_(2)还原为C_(2)产物以及优越的可充电Zn-CO_(2)电池性能
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作者 项东 李坤振 +3 位作者 苗康华 龙冉 熊宇杰 康雄武 《物理化学学报》 SCIE CAS 2024年第8期43-46,共4页
有机分子功能化是一种有前景的策略,用于调控电化学CO_(2)还原反应(eCO_(2)RR)的C_(2+)产物选择性和活性。然而,我们对于电化学CO_(2)还原调控机制的分子水平理解仍然不够清晰。在本文中,我们成功制备了铜纳米颗粒,并使用一系列胺类衍生... 有机分子功能化是一种有前景的策略,用于调控电化学CO_(2)还原反应(eCO_(2)RR)的C_(2+)产物选择性和活性。然而,我们对于电化学CO_(2)还原调控机制的分子水平理解仍然不够清晰。在本文中,我们成功制备了铜纳米颗粒,并使用一系列胺类衍生物(如十六胺(HAD)、N-甲基十六胺(N-MHDA)、十六烷基二甲胺(HDDMA)和十六酰胺(PMM))对其进行功能化,以系统地研究胺表面活性剂分子结构对eCO_(2)RR选择性和活性的影响。结果表明,HDA的功能化可以将C_(2)产物和C_(2)H_(4)的法拉第效率(FE)提高至73.5%和46.4%,并且在−0.9 V vs.RHE(可逆氢电极)电位下,C_(2)产物的分电流密度为131.4 mA·cm^(−2)。理论研究发现,HDA通过与CO_(2)和eCO_(2)RR中间体之间的氢键相互作用,富集了^(*)CO_(2)、^(*)CO和其他反应中间体,降低了CO―CHO耦合反应的动力学能垒,从而促进了eCO_(2)RR向C_(2)产物的转化。当胺基的H原子被甲基取代后,氢键相互作用减弱,竞争的析氢反应加剧。PMM通过Cu―O键与Cu表面发生键合,而不是通过Cu―N键,导致Cu-PMM更倾向于产乙醇。原位拉曼光谱显示,在Cu-HDA表面,CO主要吸附在Cu的顶位吸附位点上,与在Cu表面上的桥式吸附不同,这可能是因为前者表面对CO的富集引发了CO的吸附构型变化。HDA功能化还提高了Cu催化剂的表面pH。基于Cu-HDA组装的可充电Zn-CO_(2)电池在放电电流密度为16 mA∙cm^(−2)时,最大功率密度为6.48 mW∙cm^(−2),并具有长达60 h的良好充放电稳定性。本研究的重点在于通过在分子水平上调节Cu基材料的CO_(2)RR活性和选择性,促进CO_(2)-C_(2)的转化,这可能为提高C_(2)产物的产率提供新的见解。 展开更多
关键词 二氧化碳还原 CO―CHO耦合 有机分子功能化 原位拉曼 C_(2)产物 Zn-CO_(2)电池
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Pd-Ag alloy hollow nanostructures with interatomic charge polarization for enhanced electrocatalytic formic acid oxidation 被引量:12
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作者 Dong Liu Maolin Xie +7 位作者 Chengming wang Lingwen Liao Lu Qiu Jun Ma Hao Huang Ran Long Jun Jiang yujie xiong 《Nano Research》 SCIE EI CAS CSCD 2016年第6期1590-1599,共10页
Formic acid oxidation is an important electrocatalytic reaction in proton- exchange membrane (PEM) fuel cells, in which both active sites and species adsorption/activation play key roles. In this study, we have deve... Formic acid oxidation is an important electrocatalytic reaction in proton- exchange membrane (PEM) fuel cells, in which both active sites and species adsorption/activation play key roles. In this study, we have developed hollow Pd-Ag alloy nanostructures with high active surface areas for application to electrocatalytic formic acid oxidation. When a certain amount of Ag is incorporated into a Pd lattice, which is already a highly active material for formic acid oxidation, the electrocatalytic activity can be significantly boosted. As indicated by theoretical simulations, coupling between Pd and Ag induces polarization charges on Pd catalytic sites, which can enhance the adsorption of HCO0* species. As a result, the designed electrocatalysts can achieve reduced Pd usage and enhanced catalytic properties at the same time. This study represents an approach that simultaneously fabricates hollow structures to increase the number of active sites and utilizes interatomic interactions to tune species adsorption/ activation towards improved electrocatalytic performance. 展开更多
关键词 PALLADIUM SILVER ELECTROCATALYSIS formic add oxidation hollow nanostructures
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Recent progress on advanced design for photoelectrochemical reduction of CO_2 to fuels 被引量:25
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作者 Ning Zhang Ran Long +1 位作者 Chao Gao yujie xiong 《Science China Materials》 SCIE EI CSCD 2018年第6期771-805,共35页
The energy crisis and global warming become severe issues. Solar-driven CO2 reduction provides a promising route to confront the predicaments, which has received much attention. The photoelectrochemical(PEC) process... The energy crisis and global warming become severe issues. Solar-driven CO2 reduction provides a promising route to confront the predicaments, which has received much attention. The photoelectrochemical(PEC) process,which can integrate the merits of both photocatalysis and electrocatalysis, boosts splendid talent for CO2 reduction with high efficiency and excellent selectivity. Recent several decades have witnessed the overwhelming development of PEC CO2 reduction. In this review, we attempt to systematically summarize the recent advanced design for PEC CO2 reduction. On account of basic principles and evaluation parameters, we firstly highlight the subtle construction for photocathodes to enhance the efficiency and selectivity of CO2 reduction, which includes the strategies for improving light utilization, supplying catalytic active sites and steering reaction pathway.Furthermore, diversiform novel PEC setups are also outlined.These exploited setups endow a bright window to surmount the intrinsic disadvantages of photocathode, showing promising potentials for future applications. Finally, we underline the challenges and key factors for the further development of PEC CO2 reduction that would enable more efficient designs for setups and deepen systematic understanding for mechanisms. 展开更多
关键词 PHOTOELECTROCATALYSIS CO2 reduction light utilization SEMICONDUCTOR SELECTIVITY
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2020 roadmap on pore materials for energy and environmental applications 被引量:6
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作者 Zengxi Wei Bing Ding +11 位作者 Hui Dou Jorge Gascon Xiang-Jian Kong yujie xiong Bin Cai Ruiyang Zhang Ying Zhou Mingce Long Jie Miao Yuhai Dou Ding Yuan Jianmin Ma 《Chinese Chemical Letters》 SCIE CAS CSCD 2019年第12期2110-2122,共13页
Porous materials have attracted great attention in energy and environment applications,such as metal organic frameworks(MOFs),metal aerogels,carbon aerogels,porous metal oxides.These materials could be also hybridized... Porous materials have attracted great attention in energy and environment applications,such as metal organic frameworks(MOFs),metal aerogels,carbon aerogels,porous metal oxides.These materials could be also hybridized with other materials into functional composites with superior properties.The high specific area of porous materials offer them the advantage as hosts to conduct catalytic and electrochemical reactions.On one hand,catalytic reactions include photocatalytic,p ho toe lectrocatalytic and electrocatalytic reactions over some gases.On the other hand,they can be used as electrodes in various batteries,such as alkaline metal ion batteries and electrochemical capacitors.So far,both catalysis and batteries are extremely attractive topics.There are also many obstacles to overcome in the exploration of these porous materials.The research related to porous materials for energy and environment applications is at extremely active stage,and this has motivated us to contribute with a roadmap on ’porous materials for energy and environment applications’. 展开更多
关键词 Metal organic frameworks Zeolitic imidazolate frameworks Covalent organic frameworks AEROGELS Photocatalysis PHOTOELECTROCATALYSIS ELECTROCATALYSIS Metal-ion batteries Electrochemical capacitors
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Hydriding Pd cocatalysts: An approach to giant enhancement on photocatalytic CO2 reduction into CH4 被引量:5
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作者 Yuzhen Zhu Chao Gao +5 位作者 Song Bai Shuangming Chen Ran Long Li Song Zhengquan Li yujie xiong 《Nano Research》 SCIE EI CAS CSCD 2017年第10期3396-3406,共11页
Photocatalytic reduction of CO2 into high value-added CH4 is a promising solution for energy and environmental crises. Integrating semiconductors with cocatalysts can improve the activities for photocatalytic CO2 redu... Photocatalytic reduction of CO2 into high value-added CH4 is a promising solution for energy and environmental crises. Integrating semiconductors with cocatalysts can improve the activities for photocatalytic CO2 reduction; however, most metal cocatalysts mainly produce CO and H2. Herein, we report a cocatalyst hydridation approach for significantly enhancing the photocatalytic reduction of CO2 into CH4. Hydriding Pd cocatalysts into PdH0.43 played a dual role in performance enhancement. As revealed by our isotopic labeling experiments, the PdH0.43 hydride cocatalysts reduced H2 evolution, which suppressed the H2 production and facilitated the conversion of the CO intermediate into the final product: CH4. Meanwhile, hydridation promoted the electron trapping on the cocatalysts, improving the charge separation. This approach increased the photocatalytic selectivity in CH4 production from 3.2% to 63.6% on Pd{100} and from 15.6% to 73.4% on Pd{111}. The results provide insights into photocatalytic mechanism studies and introduce new opportunities for designing materials towards photocatalytic CO2 conversion. 展开更多
关键词 photocatalysis COCATALYST palladium hydride carbon dioxide methane
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Highly efficient overall urea electrolysis via single-atomically active centers on layered double hydroxide 被引量:5
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作者 Huachuan Sun Linfeng Li +10 位作者 Hsiao-Chien Chen Delong Duan Muhammad Humayun Yang Qiu Xia Zhang Xiang Ao Ying Wu Yuanjie Pang Kaifu Huo Chundong Wang yujie xiong 《Science Bulletin》 SCIE EI CAS CSCD 2022年第17期1763-1775,共13页
Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and ... Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and urea-rich wastewater purification;however,it remains a challenge to achieve overall urea electrolysis with high efficiency.Herein,we report a multifunctional electrocatalyst termed as Rh/Ni V-LDH,through integration of nickel-vanadium layered double hydroxide(LDH)with rhodium single-atom catalyst(SAC),to achieve this goal.The electrocatalyst delivers high HER mass activity of0.262 A mg^(-1) and exceptionally high turnover frequency(TOF)of 2.125 s^(-1) at an overpotential of100 m V.Moreover,exceptional activity toward urea oxidation is addressed,which requires a potential of 1.33 V to yield 10 mA cm^(-2),endorsing the potential to surmount the sluggish OER.The splendid catalytic activity is enabled by the synergy of the Ni V-LDH support and the atomically dispersed Rh sites(located on the Ni-V hollow sites)as evidenced both experimentally and theoretically.The selfsupported Rh/Ni V-LDH catalyst serving as the anode and cathode for overall urea electrolysis(1 mol L^(-1) KOH with 0.33 mol L^(-1) urea as electrolyte)only requires a small voltage of 1.47 V to deliver 100 mA cm^(-2) with excellent stability.This work provides important insights into multifunctional SAC design from the perspective of support sites toward overall electrolysis applications. 展开更多
关键词 Single-atomically active centers Layer double hydroxide Hydrogen evolution reaction Overall urea electrolysis High turnover frequency
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Crystal phase engineering on photocatalytic materials for energy and environmental applications 被引量:3
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作者 Song Bai Chao Gao +1 位作者 Jingxiang Low yujie xiong 《Nano Research》 SCIE EI CAS CSCD 2019年第9期2031-2054,共24页
Crystal phase engineering on photocatalytic materials is a subfield of photocatalysis with intensive research,which has been proven as a:versatile approach to maneuver their performance for applications in energy-and ... Crystal phase engineering on photocatalytic materials is a subfield of photocatalysis with intensive research,which has been proven as a:versatile approach to maneuver their performance for applications in energy-and environment-related fields.In this article,the state-of-the-art progress on phase-e ngin eered photocatalytic materials is reviewed.Firstly,we discuss the phase engin eeri ng on pristi ne semic on ductor photocatalysts,in which the phase-dependent light absorption,charge transfer and separation,and surface reaction behaviors in photocatalytic processes are summarized,respectively.Based on the elucidated mechanisms,the implementation of phase junctions in photocatalytic reactions is then presented.As a focus,we highlight the rational design of phase junctions toward steering the charge kinetics for enhanced photocatalytic and photoelectrocatalytic performance.Moreover,the crystal phase engineering on semiconductor-based hybrid photocatalysts is also in troduced,which un derli nes the importa nee of choosi ng a suitable phase for semic on ductor comp orients and co-catalysts as well as the synergism of differe nt semico nductor phases for improved photocatalytic performa nee.Fin ally,the challe nges and perspectives in this research field are proposed.In this review,particular emphasis is placed on establishing a linkage between crystal phase and photocatalytic activity to develop a structure-activity guide.Based on the guide,a framework is suggested for future research on the rational phase design of photocatalysts for improved performance in energy and environmental applications. 展开更多
关键词 PHOTOCATALYSIS CRYSTAL phase CHARGE KINETICS ARCHITECTURAL design energy environment
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Working-in-tandem mechanism of multi-dopants in enhancing electrocatalytic nitrogen reduction reaction performance of carbon- based materials 被引量:3
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作者 Wenqing Zhang Keke Mao +11 位作者 Jingxiang Low Hengjie Liu Yanan Bo Jun Ma Qiaoxi Liu Yawen Jiang Jiuzhong Yang Yang Pan Zeming Qi Ran Long Li Song yujie xiong 《Nano Research》 SCIE EI CSCD 2021年第9期3234-3239,共6页
Developing carbon-based electrocatalysts with excellent N2 adsorption and activation capability holds the key to achieve highly efficient nitrogen reduction reaction(NRR)for reaching its practical application.Here,we ... Developing carbon-based electrocatalysts with excellent N2 adsorption and activation capability holds the key to achieve highly efficient nitrogen reduction reaction(NRR)for reaching its practical application.Here,we report a highly active electrocatalyst--metal-free pyrrolic-N dominated N,S co-doped carbon(pyrr-NSC)for NRR.Based on theoretical and experimental results,it is confirmed that the N and S-dopants practice a working-in-tandem mechanism on pyrr-NSC,where the N-dopants are utilized to create electropositive C sites for enhancing N2 adsorption and the S-dopants are employed to induce electron backdonation for facilitating N2 activation.The synergistic effect of the pyrrolic-N and S-dopants can also suppress the irritating hydrogen evolution reaction,further boosting the NRR performance.This work gives an indication that the combination of two different dopants on electrocatalyst can enhance NRR performance by working in the two tandem steps-the adsorption and activation of N2 molecules,providing a new strategy for NRR electrocatalyst design. 展开更多
关键词 N2 reduction reaction metal-free catalyst heteroatoms doping asymmetric charge distribution ELECTROCATALYSIS
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