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Biosynthetic CdS-Thiobacillus thioparus hybrid for solar-driven carbon dioxide fixation

Nano Research 2023年第4期16卷 4531-4538页

作者： Guangyu Liu Feng Gao Hongwei Zhang Lei Wang Chao Gao yujie xiong Hefei National Laboratory for Physical Sciences at the Microscale and School of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei 230026China Institute of Energy Hefei Comprehensive National Science Center350 Shushanhu Rd.Hefei 230031China State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

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 ***,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 ***,we present an inorganic-biological hybrid system composed of obligate autotrophic bacteria Thiobacillus 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 *** optimized interface between CdS NPs and *** formed by biological precipitation plays an essential role for *** efficiently receiving photogenerated electrons from CdS NPs and thus changing the autotrophic way from chemoautotroph to *** a result,the *** 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 *** work provides significant inspiration for the further exploration of the solar-driven self-replicating biocatalytic system to achieve CO_(2)fixation and conversion.

关键词： biohybrids solar-driven CO_(2)fixation carbon cycle autotrophic bacteria Thiobacillus thioparus cadmium sulfide

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康复床结合神经肌电刺激在脓毒症肺损伤中的应用

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中国现代医生 2024年第6期62卷 24-26页

作者：熊玉洁江榕刘洪所熊淑琴洪慧南昌大学第一附属医院重症医学科江西南昌336000 南昌大学第一附属医院康复科江西南昌3360001

目的探讨在脓毒症急性肺损伤患者康复中应用康复床联合神经肌电刺激方案的临床效果。方法选取南昌大学第一附属医院重症医学科(intensive care unit,ICU)2020年6月至2022年1月收治的79例脓毒症并急性肺损伤患者作为研究对象。采用随机... 详细信息

目的探讨在脓毒症急性肺损伤患者康复中应用康复床联合神经肌电刺激方案的临床效果。方法选取南昌大学第一附属医院重症医学科(intensive care unit,ICU)2020年6月至2022年1月收治的79例脓毒症并急性肺损伤患者作为研究对象。采用随机数字表法将患者分为试验组(n=43)和对照组(n=36)。对照组患者给予常规康复治疗干预,试验组患者增加使用康复床和神经肌电刺激,比较两组患者的康复效果。结果试验组患者的无创机械通气时间、ICU入住时间、住院时间均短于对照组(P<0.05)。试验组患者干预后20d、30d的肌力评定量表评分均高于对照组(P<0.05)。试验组患者干预后30d的改良Barthel指数评分高于对照组(P<0.05)。结论康复床联合神经肌电刺激康复治疗方案可有效缩短脓毒症急性肺损伤患者的康复进程并提高康复效果。

关键词：脓毒症急性肺损伤康复床神经肌电刺激

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Control of selectivity in organic synthesis via heterogeneous photocatalysis under visible light

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Nano Research Energy 2022年第1期1卷 90-109页

作者： Yitao Dai yujie xiong Suzhou Institute for Advanced Research University of Science and Technology of ChinaSuzhou 215123China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China

Organic synthesis driven by heterogeneous catalysis is a central research theme to both fundamental research and industrial production of fine ***,the employment of stoichiometric strong oxidizing or reducing reagents(e.g.,K_(2)Cr_(2)O_(7) and LiAlH_(4))and harsh reaction conditions(e.g.,high temperature and pressure)always leads to the products of overreaction and other by-product residues(e.g.,salt and acid waste).Thus the poor control of product selectivity and tremendous energy consumption result in the urgent demand to develop novel technologies for heterogeneous *** the current global theme of development in CO_(2) reduction and sustainable energy utilization,one promising protocol is heterogeneous *** enables sustainable solar-to-chemical energy conversion under mild conditions(e.g.,room temperature,ambient pressure,and air as the oxidant)and offers unique reaction pathways for improved selectivity *** accurately tailor the selectivity of desired products,the electronic structure(e.g.,positions of valence-band maximum and conduction-band minimum),geometric structure(e.g.,nanorod,nanosheet,and porous morphology),and surface chemical micro-environment(e.g.,vacancy sites and co-catalysts)of heterogeneous photocatalysts require rational design and *** this review,we will briefly analyze some effective photocatalytic systems with the excellent regulation ability of product selectivity in organic transformations(mainly oxidation and reduction types)under visible light irradiation,and put forward opinions on the optimal fabrication of nanostructured photocatalysts to realize selective organic synthesis.

关键词： organic synthesis selectivity control heterogeneous photocatalysis photocatalyst design visible light irradiation

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Recent progress in electrochemical C–N coupling reactions

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eScience 2023年第1期3卷 26-37页

作者： Yuan Zhong Hailong xiong Jingxiang Low Ran Long yujie xiong Hefei National Research Center for Physical Sciences at the Microscale School of Chemistry and Materials ScienceNational Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefeiAnhui 230026China Institute of Energy Hefei Comprehensive National Science Center350 ShushanhuRd.HefeiAnhui 230031China

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 *** related reaction mechanisms and potential design principles for advanced electrocatalysts are *** addition,the effects of different reactors,including H-cells,membrane-based flow reactors,and membrane electrode assembly electrolyzers,on the coupling reactions are ***,the current challenges and future opportunities in this field are *** aim to provide an up-to-date overview of the electrochemical C–N coupling system to advance progress toward its practical application.

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

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Nano Research 2023年第5期16卷 6728-6735页

作者： Jiayi Li Xin Mao Wanbing Gong Xinyu Wang Yawen Jiang Ran Long Aijun Du yujie xiong National Synchrotron Radiation Laboratory Hefei National Research Center for Physical Sciences at the MicroscaleSchool of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei 230026China Institute of Energy Hefei Comprehensive National Science CenterHefei 230031China School of Chemistry Physics and Mechanical EngineeringScience and Engineering FacultyQueensland University of TechnologyGardens Point CampusBrisbaneQLD 4001Australia

The thermodynamically favorable electrocatalytic oxidation coupled with hydrogen evolution reaction(HER)is considered as a sustainable and promising ***,it remains a great challenge due to the lack of simple,cheap,highefficient ***,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 ***,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 *** 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 *** 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 *** 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.

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

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Chinese Chemical Letters 2023年第3期34卷 460-464页

作者： Kun Chen Wei Zhang Yu Bai Wanbing Gong Ning Zhang Ran Long yujie xiong a School of Chemistry and Materials Science Frontiers Science Center for Planetary Exploration and Emerging TechnologiesNational Synchrotron Radiation Laboratoryand Experimental Center of Engineering and Material SciencesUniversity of Science and Technology of ChinHefei 230026China Key Laboratory of Magnetic Materials at Universities of Inner Mongolia Autonomous Region Baotou Teachers’CollegeBaotou 014030China Department of Applied Physics The Hong Kong Polytechnic UniversityHong Kong 999077China Institute of Energy Hefei Comprehensive National Science CenterHefei 230031China

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.

关键词： Electrosynthesis Benzylamine dehydrogenation Coupling Hydrogen evolution Cobalt cyclotetraphosphate

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Highly Efficient Photocatalytic CO_(2) Methanation over Ru-Doped TiO_(2) with Tunable Oxygen Vacancies

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Chinese Journal of Structural Chemistry 2022年第12期41卷 43-50页

作者： Zheyue Li Di Wu Wanbing Gong Jiayi Li Shuaikang Sang Hengjie Liu Ran Long yujie xiong Hefei National Research Center for Physical Sciences at the Microscale School of Chemistry and Materials ScienceNational Synchrotron Radiation LaboratorySchool of Nuclear Science and TechnologyUniversity of Science and Technology of ChinaHefei 230026China Institute of Energy Hefei Comprehensive National Science Center350 Shushanhu Rd.Hefei 230031China

Solar-driven CO_(2) methanation is an imperative and promising approach to relieve the global warming and environmental crisis,yet remains a great challenge due to the low reaction efficiency,unsatisfactory selectivity and poor *** this work,we demonstrate a facile and efficient strategy to prepare Ru-doped TiO_(2) photocatalyst with tunable oxygen vacancies using the ascorbic acid as a reducing agent for the CO_(2) methanation *** optimal Ru-TiO_(2)-OV-50 exhibits a remarkable CH4production rate of 81.7 mmol g^(-1)h^(-1)with a 100%CH4selectivity under a 1.5 W cm^(-2)light illumination,which is significantly higher than commercial Ru/TiO_(2)and other reported *** reveal that the superior photocatalytic CO_(2) methanation performance is mainly due to the synergistic effect of Ru doping and TiO_(2) with tunable oxygen ***,the light rather than thermal effect is confirmed as the main influencing factor by experimental *** addition,in situ spectroscopic technology is performed to investigate the CO_(2) methanation reaction *** work will open an avenue to design and prepare highly efficient photocatalyst with tunable oxygen vacancies for CO_(2) conversion and other related applications.

关键词： photocatalysis CO_(2)methanation metal doping titanium oxide oxygen vacancies

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Atomically dispersed N-coordinated Fe-Fe dual-sites with enhanced enzyme-like activities

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Nano Research 2022年第2期15卷 959-964页

作者： Lei Jiao Wei Ye Yikun Kang Yu Zhang Weiqing Xu Yu Wu Wenling Gu Weiyu Song yujie xiong Chengzhou Zhu Key Laboratory of Pesticide and Chemical Biology of Ministry of Education International Joint Research Center for Intelligent Biosensing Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan 430079China College of Material Chemistry and Chemical EngineeringHangzhou Normal UniversityHangzhou 311121China State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing 102249China Hefei National Laboratory for Physical Sciences at the Microscale Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)School of Chemistry and Materials Scienceand National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China

Replacement of enzymes with nanomaterials such as atomically dispersed metal catalysts is one of the most crucial steps in addressing the challenges in *** the breakthroughs of single-atom catalysts in enzyme-mimicking,a fundamental investigation on the development of an instructional strategy is still required for mimicking biatomic/multiatomic active sites in natural enzymes and constructing synergistically enhanced metal atom active ***,Fe_(2)NC catalysts with atomically dispersed Fe-Fe dual-sites supported by the metal-organic frameworks-derived nitrogen-doped carbon are employed as biomimetic catalysts to perform proof-of-concept *** effect of Fe atom number toward typical oxidase(cytochrome C oxidase,NADH oxidase,and ascorbic acid oxidase)and peroxidase(NADH peroxidase and ascorbic acid peroxidase)activities is systematically evaluated by experimental and theoretical investigations.A peroxo-like O_(2) adsorption in Fe_(2)NC nanozymes could accelerate the O-O activation and thus achieve the enhanced enzyme-like *** work achieves the vivid simulation of the enzyme active sites and provides the theoretical basis for the design of high-performance *** a concept application,a colorimetric biosensor for the detection of S^(2-) in tap water is established based on the inhibition of enzyme-like activity of Fe_(2)NC nanozymes.

关键词： nanozymes atomically dispersed dual-metal sites oxidase-like activities single-atom catalysis sensors

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Identification and Design of Active Sites on Photocatalysts for the Direct Artificial Carbon Cycle

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Accounts of Materials Research 2022年第3期3卷 331-342页

作者： Jingxiang Low Jun Ma Jun Wan Wenbin Jiang yujie xiong Hefei National Laboratory for Physical Sciences at the Microscale School of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefeiAnhui 230026China Multidisciplinary Platform of Advanced Engineering Chemical Engineering DisciplineSchool of EngineeringMonash UniversityBandar Sunway 47500 SelangorMalaysia

CONSPECTUS:Imitating the natural carbon cycle,the utilization of the carbon-based greenhouse gases(i.e.,carbon dioxide(CO_(2))and methane(CH_(4)))from the atmosphere as the carbon feedstocks for valuable fuel and chemical production represents a prospective strategy for achieving the sustainable development of human *** light of this,photocatalytic CO_(2)/CH_(4)conversions,which can directly harvest solar energy for the production of valuable fuels and chemicals,show gigantic potential for closing the loop of the artificial carbon *** the past several decades,immense progress has been made in this field,showing its practical ***,the photocatalytic conversion efficiency and selectivity of such reactions remain *** that the photocatalytic reaction is intimately related to the surface catalytic reaction on the active sites of the photocatalysts,the active site design has been proven to be effective for optimizing photocatalytic performance,yet the lack of effective techniques for the identification of the active sites,which is normally at the molecular level,greatly limits its potential in ***,with the rapid expansion in the field of materials science,a large number of advanced characterization techniques have been developed,equipping the materials scientist and chemist with powerful tools for unveiling the mask of the active sites on the ***,the active site design for the photocatalysts has undergone a ***,the identification and design of active sites have emerged as hot topics in catalysis and are expected to push forward development in the field of the artificial carbon cycle.

关键词： dioxide catalysis Active

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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

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Nano Research 2023年第4期16卷 4494-4498页

作者： Chaohua He Delong Duan Jingxiang Low Yu Bai Yawen Jiang Xinyu Wang Shuangming Chen Ran Long Li Song yujie xiong Hefei National Laboratory for Physical Sciences at the Microscale Frontiers Science Center for Planetary Exploration and Emerging TechnologiesSchool of Chemistry and Materials Scienceand National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China Hefei Comprehensive National Science Center 350 Shushanhu Rd.Hefei 230031China

Cu-based electrocatalysts have provoked much attention for their high activity and selectivity in carbon dioxide(CO_(2))conversion into multi-carbon ***,during the electrochemical reaction,Cu catalysts inevitably undergo surface reconstruction whose impact on CO_(2)conversion performance remains *** 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)*** 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 *** 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 ***,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**** 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.

关键词： CO_(2)electroreduction reaction surface reconstruction high-index facets ethylene(C_(2)H_(4)) Cu catalysts

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