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Defect engineered electrocatalysts for C-N coupling reactions toward urea synthesis

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Chinese Chemical Letters 2024年第8期35卷 7-14页

作者： Shengkai Li Yuqin Zou Chen Chen Shuangyin Wang zhao-qing liu Guangzhou Key Laboratory for Clean Energy and Materials/Key Laboratory for Water Quality and Conservation of the Pearl River Delta Ministry of EducationGuangzhou UniversityGuangzhou 510006China State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of EducationHunan UniversityChangsha 410082China

Urea is extensively used in agriculture and chemical industry,and it is produced on an industrial scale from CO_(2)and Haber-Bosch NH_(3)under relatively high temperature and high pressure conditions,which demands high energy input and generates masses of carbon *** conversion of CO_(2)and N sources(such as NO_(2)^(−),NO_(3)^(−),and N_(2))through electrocatalytic reactions under ambient conditions is a promising alternative to realize efficient urea *** note,the design of electrocatalyst is one of the key factors that can improve the efficiency and selectivity of C-N coupling *** engineer-ing is an intriguing strategy for regulating the electronic structure and charge density of electrocatalysts,which endows electrocatalysts with excellent physicochemical properties and optimized adsorption en-ergy of the reaction intermediates to reduce the kinetic *** this minireview,recent advances of defect engineered electrocatalysts in urea electrosynthesis from CO_(2)and various N reactants are firstly *** discussions of C-N coupling in these advances are presented,with the aim of directing future investigations on improving the urea ***,the prospects and challenges of de-fect engineered electrocatalysts for urea synthesis are *** overview is expected to provide in-depth understanding of structure-reactivity relationship and shed light on future electrocatalytic C-N coupling reactions.

关键词： Electrocatalysis Defective electrocatalyst Co-reduction C-N coupling Urea synthesis

分层干预联合饮食指导在急性上消化道出血患者中的应用效果

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黔南民族医专学报 2024年第2期37卷 212-215页

作者：赵柳青李薇薇商丘市第一人民医院河南商丘476000

目的:探讨分层干预联合饮食指导应用于急性上消化道出血的治疗效果。方法:根据随机数字表法将2021年6月至2022年6月在本院接受治疗的82例急性上消化道出血患者分为对照组(41例)与联合组(41例);对照组患者进行饮食指导,联合组在对照组的... 详细信息

目的:探讨分层干预联合饮食指导应用于急性上消化道出血的治疗效果。方法:根据随机数字表法将2021年6月至2022年6月在本院接受治疗的82例急性上消化道出血患者分为对照组(41例)与联合组(41例);对照组患者进行饮食指导,联合组在对照组的基础上联合采用分层干预;比较两组患者的自我管理评分、营养指标及预后不良反应情况。结果:3个月后随访的结果显示,联合组患者的饮食、用药、病情监测、日常生活评分以及总分、血红蛋白(Hb)、转铁蛋白(TRF)、血尿素氮(BUN)水平明显高于对照组(P<0.05);不良反应发生率明显低于对照组(P<0.05)。结论:分层干预联合饮食指导应用于急性上消化道出血患者的预后情况较好,可以明显改善患者的营养状况,增强患者的自我管理能力。

关键词：急性上消化道出血饮食指导分层干预自我管理

Landfill leachate production, quality and recirculation treatment in northeast China

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Journal of Environmental Sciences 2006年第4期18卷 625-628页

作者： zhao qing-liang liu Xue-yan QI Xu-dong liu Zhi-gang School of Municipal and Environment Engineering Harbin Institute of Technology Harbin 150090 China

Landfill leachate recirculation treatment process is a promising and economic way in northeast China due to the distinct season variation. In order to study the impact of recirculation on leachate production and its quality, two simulated sanitary landfill reactors, one with leachate recirculation and the other without, were placed outdoor in Harbin. The two-year experimental results indicated that leachate production was reduced by 86% with leachate recirculation and less or no facility for leachate treatment required. Recirculation could improve the leachate quality dramatically with lower COD, SS, NF4-N and higher pH level. Recirculation also could enhance waste degradation and stabilization and improve the efficiency of landfill. This study confirmed that leachate recirculation was a very feasible way for on-site landfill leachate treatment in cold areas.

关键词： cold area sanitary landfill leachate recirculation solid waste

Development and validation of depletion code system IMPC Burnup for ADS

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Nuclear Science and Techniques 2019年第3期30卷 65-74页

作者： zhao-qing liu Ze-Long zhao Yong-Wei Yang Yu-Cui Gao Hai-Yan Meng qing-Yu Gao Institute of Modern Physics Chinese Academy of Sciences School of Nuclear Science and Technology University of Chinese Academy of Sciences

Depletion calculation is important for studying the transmutation efficiency of minor actinides and longlife fission products in accelerator-driven subcritical reactor system(ADS). Herein the Python language is used to develop a burnup code system called IMPC-Burnup by coupling FLUKA, OpenMC, and ORIGEN2. The program is preliminarily verified by OECD-NEA pin cell and IAEAADS benchmarking by comparison with experimental values and calculated results from other studies. Moreover,the physics design scheme of the CIADS subcritical core is utilized to test the feasibility of IMPC-Burnup program in the burnup calculation of ADS system. Reference results are given by the COUPLE3.0 program. The results of IMPC-Burnup show good agreement with those of COUPLE3.0. In addition, since the upper limit of the neutron transport energy for OpenMC is 20 MeV, neutrons with energies greater than 20 MeV in the CIADS subcritical core cannot be transported; thus, an equivalent flux method has been proposed to consider neutrons above 20 MeV in the OpenMC transport calculation. The results are compared to those that do not include neutrons greater than 20 MeV. The conclusion is that the accuracy of the actinide nuclide mass in the burnup calculation is improved when the equivalent flux method is used. Therefore, the IMPC-Burnup code is suitable for burnup analysis of the ADS system.

关键词： ADS-coupled proton-neutron transport Burnup calculation IMPC-Burnup FLUKA OpenMC ORIGEN2

S, N co-doped carbon nanotube-encapsulated core-shelled CoS2@Co nanoparticles： efficient and stable bifunctional catalysts for overall water splitting

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Science Bulletin 2018年第17期63卷 1130-1140页

作者： Jing-Yu Wang Ting Ouyang Nan Li Tianyi Ma zhao-qing liu School of Chemistry and Chemical Engineering/Key Laboratory for Water Quality and Conservation of the Pearl River Delta Ministry of Education Guangzhou UniversityGuangzhou 510006 China Discipline of Chemistry University of Newcastle Newcastle NSW 2308 Australia School of Chemical Engineering University of Adelaide Adelaide SA 5005 Australia

Hydrogen, serving as a clean, sustainable energy source, may be mainly produced from electrolysis water. Herein, we report cobalt disulphide encapsulated in self-catalyzed carbon nanotubes （S, N-CNTs/ CoS2@Co） serving as a bifunctional catalyst, which exhibits excellent hydrogen evolution reaction perfor-mance （10.0 mAcm^-2 at 0.112 V, and low Tafel slope for 104.9 mV dec^-1 ） and oxygen evolution reaction performance （10.0 mAcm^-2 at 1.57 V, and low Tafel slope for 76.1 mV dec^-1）, meanwbile with a strong stability at various current densities. In-depth study reveals that the excellent catalytic properties can be mainly attributed to the increased catalytic sites induced by S, N co-doping, the improved electronic con-ductivity derived from the carbon nanotubes, and Mott-Schottky effect between the metal cobalt and semiconductive cobalt disulfide. Notably, when the bifunctional catalysts are applied to overall water splitting, a low potential of 1.633 V at the current density of 10.0 mAcm^-2 is achieved, which can com-pete with the precious metal catalyst benchmarks in alkaline media, demonstrating its promising prac-ticability in the realistic water splitting application. This work elucidates a practicable way to the design of transition metal and nano-carbon composite catalysts for a broad application in the fields of energy chemistry.

关键词： Core-shell structure Hydrogen evolution Oxygen evolution Bifunctional catalyst Overall water splitting

Enhanced electron transport through two-dimensional Ti_(3)C_(2) in dye-sensitized solar cells

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Rare Metals 2022年第9期41卷 3078-3085页

作者： Gang Wang Li-Jiao Ma Bing-Xin Lei Heng Wu zhao-qing liu Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province Key Laboratory of Electrochemical Energy Storage and Light Energy Conversion Materials of Haikou CitySchool of Chemistry and Chemical EngineeringHainan Normal UniversityHaikou571158China School of Materials and Environment Guangxi University for NationalitiesNanning530006China Guangzhou Key Laboratory for Clean Energy and Materials Huangpu Hydrogen Innovation CenterInstitute of Clean Energy and MaterialsSchool of Chemistry and Chemical EngineeringGuangzhou UniversityGuangzhou510006China

Two-dimensional(2D)Ti_(3)C_(2) material has a wide range of photovoltaic applications due to its unique electronic,optical,and plasmonic ***,we present a series of Ti_(3)C_(2)(0,0.6,0.8;wt%)nanosheets-modified P25 nanoparticles as photoanode films for dye-sensitized solar cells(DSSCs).The DSSC based on P25 and 0.6 wt%Ti_(3)C_(2) photoanode achieves a fairly good efficiency(9.22%),which greatly exceeds the counterpart based on the pure P25(7.16%).Benefiting from high light scattering and metallic electrical conductivity of Ti_(3)C_(2) additive,the P25/Ti_(3)C_(2)-based DSSC exhibits a superior behavior of controlling photogenerated charge recombination compared with pure P25 one.

关键词： Ti3C2 Conductivity Charge transfer Dyesensitized solar cells

Single-phase bimetal sulfide or metal sulfide heterojunction:Which one is better for reversible oxygen electrocatalyst?

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Journal of Energy Chemistry 2022年第11期31卷 420-428,I0012页

作者： Jingjing Cai Huijun liu Yulin Luo Yuqing Xiong Lizhu Zhang Sheng Wang Kang Xiao zhao-qing liu School of Chemistry and Chemical Engineering/Institute of Clean Energy and Materials/Key Laboratory for Clean Energy and Materials Guangzhou UniversityGuangzhou 510006GuangdongChina Department of Materials Science and Engineering Northwestern UniversityEvanstonIL 60208USA

Bimetallic sulfides,integrating the merits of individual components,are ideal structures for efficient ***,for bimetallic sulfides including metal sulfide heterojunctions(MSH)and singlephase bimetallic sulfides(SBS),it is still unclear about which one has better catalytic activity toward reversible oxygen catalysis and its difference on catalytic *** this work,we demonstrate a bimetallic sulfide electrocatalyst that could transform from metal sulfide heterojunction(CoS/FeS)to single-phase bimetallic sulfide(CoFeS_(2))through a facile temperature control *** single-phase bimetallic sulfide(CoFeS_(2))affords high intrinsic activity,fast reaction kinetics and superior durability toward oxygen evolution reaction(OER)and oxygen reduction reaction(ORR).Density functional theory(DFT)simulations reveal that the(CoFeS_(2))has homogeneous electron distribution of the CoFeS_(2)structure,improves the central energy level of d band,and optimizes the O*and OOH*intermediate and efficiently reduces the energy barrier of the reaction rate-determining step(RDS).The assembled rechargeable zincair battery is more stable than the Pt/C and IrO_(2) assemblies due to the excellent electrocatalytic activity and stability of CoFeS_(2)/NC,suggesting that it has potential for use in practical applications.

关键词： Metal sulfide Sulfide heterojunction OER ORR Zinc-air batteries

Transition metal-based electrocatalysts for overall water splitting

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Chinese Chemical Letters 2021年第9期32卷 2597-2616页

作者： Xiao-Peng Li Can Huang Wen-Kai Han Ting Ouyang zhao-qing liu School of Chemistry and Chemical Engineering Institute of Clean Energy and MaterialsGuangzhou Key Laboratory for Clean Energy and MaterialsKey Laboratory for Water Quality and Conservation of the Pearl River DeltaMinistry of EducationGuangzhou UniversityGuangzhou Higher Education Mega CenterGuangzhou 510006China

Electrochemical overall water splitting is attracting a broad focus as a promising strategy for converting the electrical output of renewable resources into chemical fuels,specifically oxygen and ***,the urgent challenge in water electrolysis is to search for low-cost,high-efficiency catalysts based on earth-abundant elements as an alternative to the high-cost but effective noble metal-based *** transition metal-based catalysts are more appealing than the noble metal catalysts because of its low cost,high performance and long *** recent advances for the development in overall water splitting are reviewed in terms of transition metal-based oxides,carbides,phosphides,sulfides,and hybrids of their mixtures as hybrid bifunctional *** on different catalytic mechanisms,recent advances in their structural design,controllable synthesis,mechanistic insight,and performance-enhancing strategies are *** challenges and prospects for the future development of transition metal-based bifunctional electrocatalysts are also addressed.©2021 Chinese Chemical Society and Institute of Materia Medica,Chinese Academy of Medical Sciences.

关键词： Transition metal-based Electrocatalysts Hydrogen evolution reaction Oxygen evolution reaction Overall water splitting

Molybdenum phosphide(MoP) with dual active sites for the degradation of diclofenac in Fenton-like system

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Chinese Chemical Letters 2022年第3期33卷 1321-1324页

作者： Xiuying Li Shuangqiu Huang Huaihao Xu Yuepeng Deng Zhu Wang zhao-qing liu Key Laboratory for Water Quality and Conservation of the Pearl River Delta Ministry of EducationGuangzhou Key Laboratory for Clean Energy and MaterialsInstitute of Environmental Research at Greater BayGuangzhou UniversityGuangzhou 510006China School of Chemistry and Chemical Engineering Institute of Clean Energy and MaterialsGuangzhou Key Laboratory for Clean Energy and MaterialsKey Laboratory for Water Quality and Conservation of the Pearl River DeltaMinistry of EducationGuangzhou UniversityGuangzhou 510006China State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China

The leaching and non-recoverability of mental ions have always limited the practical application of Fenton-like processes. For the first time, we synthesized molybdenum phosphide (MoP) with dual active sites for the degradation of diclofenac (DCF) in the Fenton-like process. The DCF degradation rate constant (k) of MoP + H_(2)O_(2) process was calculated to be 0.13 min^(-1) within 40 min, indicating a highly efficient catalytic ability of MoP. In addition, this catalyst exhibits a stable structure and good activity, which could apply in a broad pH range, different ions solution and real wastewater condition. Accordingly, this efficient catalytic capability may be attributed to the presence of the metal sites Mo^(δ+) and the electron-rich sites P^(δ-) in MoP, which could induce the generation of hydroxyl radical (^(·)OH) and superoxide radical (^(·)O_(2)^(-)) through electron transfer, resulting in the effective removal of DCF. This study provides an idea for the optimization of Fenton-like technologies and environmental remediation.

关键词： MoP Dual active sites Fenton-like Diclofenac degradation