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Atomically Dispersed Zinc Active Sites Efficiently Promote the Electrochemical Conversion of N_(2) to NH_(3)

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Energy & Environmental Materials 2024年第3期7卷 175-181页

作者： Yanjiao Wei Xinyu Wang Mengjie Sun Min Ma Jian Tian minhua shao School of Materials Science and Engineering Shandong University of Science and TechnologyQingdao 266590China Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong 999077China Energy Institute and Chinese National Engineering Research Center for Control&Treatment of Heavy Metal PollutionThe Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong China

At present,the research on highly active and stable nitrogen reduction reaction catalysts is still challenging work for the electrosynthesis of ammonia(NH_(3)).Herein,we synthesized atomically dispersed zinc active sites supported on N-doped carbon nanosheets(Zn/NC NSs)as an efficient nitrogen reduction reaction catalyst,which achieves a high ammonia yield of 46.62μg h^(-1)mg^(-1)_(cat).at-0.85 V(vs RHE)and Faradaic efficiency of 95.8%at-0.70 V(vs RHE).In addition,Zn/NC NSs present great stability and selectivity,and there is no significant change in NH_(3)rate and Faradaic efficiencies after multiple *** structural characterization shows that the active center in the nitrogen reduction reaction process is the Zn-N_(4)sites in the *** calculation confirms that Zn/NC with Zn-N_(4)configuration has a lower energy barrier for the formation of^(*)NNH intermediate compared with pure N-doped carbon nanosheets(N-C NSs),thus promoting the hydrogenation kinetics in the whole nitrogen reduction reaction process.

关键词： electrocatalysis nitrogen reduction single-atom catalyst Zn-N_(4)

Toward carbon neutrality by artificial photosynthesis

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Frontiers in Energy 2024年第1期18卷 54-55页

作者： Baowen ZHOU minhua shao Sharif Md.SADAF Shuhui SUN Key Laboratory for Power Machinery and Engineering of the Ministry of Education Research Center of Renewable Synthetic FuelSchool of Mechanical EngineeringShanghai Jiao Tong UniversityShanghai 200240China Department of Chemical and Biological Engineering Energy InstituteThe Hong Kong University of Science and TechnologyHong KongChina Institut National de la Recherche Scientifique(INRS)-CenterÉnergie Matériaux Télécommunications VarennesQuebec J3X 1P7Canada

CO_(2)is not only the primary cause of climate change but also an abundant and recyclable carbon *** breakthrough in emerging disruptive technologies such as carbon capture and storage(CCS),power-to-X,and direct air capture(DAC)is fundamental to achieving carbon *** these technologies,artificial photosynthesis offers an attractive method for recycling carbon dioxide and water into fuels and chemicals using solar energy(CO_(2)+H_(2)O+sunlight→fuels+chemicals).It holds great promise for addressing the critical challenges associated with elevated CO_(2)concentrations and securing a sustainable supply of fuels and chemicals for economic sectors.

关键词： neutral holds breakthrough

Efficient C-N coupling in electrocatalytic urea generation on copper carbonate hydroxide electrocatalysts

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Journal of Energy Chemistry 2024年第6期93卷 289-298,I0008页

作者： Yinuo Wang Yian Wang Qinglan Zhao Hongming Xu Shangqian Zhu Fei Yang Ernest P.Delmo Xiaoyi Qiu Chi Song Juhee Jang Tiehuai Li Ping Gao MDanny Gu minhua shao Advanced Materials Thrust The Hong Kong University of Science and Technology(Guangzhou)Guangzhou 511400GuangdongChina Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayKowloonHong KongChina Department of Materials Science and Engineering Southern University of Science and Technology of Chin11088 Xueyuan BoulevardShenzhen 518055GuangdongChina Energy Institute and Chinese National Engineering Research Center for Control&Treatment of Heavy Metal PollutionThe Hong Kong University of Science and TechnologyKowloonHong KongChina Department of Chemistry City University of Hong KongTat Chee AvenueKowloonHong KongChina

Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of ***,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen *** thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~**** work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.

关键词： Copper carbonate hydroxide Co-reduction Urea generation C-N coupling DFT calculation

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谷固醇血症患儿临床诊疗及基因检测分析

中国麻风皮肤病杂志 2024年第3期40卷 170-175页

作者：司晨琛吴维邵敏华杨挺无锡市儿童医院皮肤科江苏无锡214000

目的:分析谷固醇血症患儿的临床表现、实验室检查、基因检测及血清植物固醇谱结果,以提高对该罕见病的诊疗水平。方法:回顾性分析2021年4月至2023年4月在无锡市儿童医院皮肤科首诊并诊断为谷固醇血症的患儿临床特征,常规生化检验结果。... 详细信息

目的:分析谷固醇血症患儿的临床表现、实验室检查、基因检测及血清植物固醇谱结果,以提高对该罕见病的诊疗水平。方法:回顾性分析2021年4月至2023年4月在无锡市儿童医院皮肤科首诊并诊断为谷固醇血症的患儿临床特征,常规生化检验结果。行全外显子测序,Sanger测序和植物固醇谱检测分析,随访1年余观察患儿临床症状变化及实验室检查指标变化。结果:3例患儿中2例以首发皮肤黄色瘤就诊。3例患儿共检测出4种基因突变,其中发现1个新突变位点为本文首报。患者1、2的ABCG8外显子发生复合杂合突变(ABCG8 NM_022437:c.1724G>A,p.G575D,ABCG8 NM_022437:c.788G>A,p.R263Q)。患者3的ABCG5外显子发生复合杂合突变(ABCG5 NM_022436.2:c.751C>T,***251*,ABCG5 NM_022436.2:c.-76C>T)。治疗前患儿1、2植物固醇谱检测高于正常水平。3例患儿均低固醇饮食,其中患儿1联合口服依哲麦布。治疗并随访1年余3例患儿的血脂水平均恢复正常;患儿1和2的植物固醇谱水平较治疗前显著降低;2例首发皮肤黄瘤患儿的黄瘤明显变平甚至消失。结论:谷固醇血症患儿常表现为关节附近的皮肤黄瘤,胆固醇升高。诊断需要基因检测及血清植物固醇谱分析证据。低植物固醇饮食、依折麦布对其治疗至关重要。

关键词：皮肤黄瘤谷固醇血症基因检测血清植物固醇谱

Investigation of cubic Pt alloys for ammonia oxidation reaction

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Nano Research 2020年第7期13卷 1920-1927页

作者： Yat Tung Chan Kumar Siddharth minhua shao Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayKowloonHong KongChina

As a promising fuel candidate,ammonia has been successtully used as anode feed in alkaline fuel ***,current technology in catalysts for ammonia electro-oxidation reaction(AOR)with respect to both cost and performance is inadequate to ensure large scale commercial application of direct ammonia fuel *** studies found that alloying Pt with different transition metals and controlling the morphology of catalysts can improve the AOR activity,and thus potentially can solve the cost ***,(100)-terminated Pt-M nanocubes(M=3d-transition metals Fe,Co,Ni,Zn)are synthesized via wet-chemistry method and their catalytic activities toward AOR are *** addition of Fe,Co,Ni and Zn elements can enhance the AOR activity due to decrease in oxophilicity of platinum and bifunctional ***-Zn exhibits the maximum mass activity and specific ativity with values of 0.41 A/mgpt and 169 mA/cm2 that are 1.6 and 1.8 times higher than Pt nanocubes,***-Fe,Pt-Co and PI-Ni nanocubes also ilustrate higher mass and specific activities compared to Pt nanocubes.

关键词： ammonia oxidation reaction electrocatalysts Pt-3d transition metal nanocubes OH adsorption

Development of organic redox-active materials in aqueous flow batteries: Current strategies and future perspectives

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SmartMat 2023年第4期4卷 85-104页

作者： Mingguang Pan minhua shao Zhong Jin State Key Laboratory of Coordination Chemistry MOE Key Laboratory of Mesoscopic ChemistryMOE Key Laboratory of High Performance Polymer Materials and TechnologyJiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjingChina Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyHong KongChina

Aqueous redox flow batteries,by using redox-active molecules dissolved in nonflammable water solutions as electrolytes,are a promising technology for grid-scale energy *** redox-active materials offer a new opportunity for the construction of advanced flow batteries due to their advantages of potentially low cost,extensive structural diversity,tunable electrochemical properties,and high natural *** this review,we present the emergence and development of organic redox-active materials for aqueous organic redox flow batteries(AORFBs),in particular,molecular engineering concepts and strategies of organic redox-active *** typical design strategies based on organic redox species for high-capacity,high-stability,and high-voltage AORFBs are outlined and *** engineering of organic redox-active molecules for high aqueous solubility,high chemical/electrochemical stability,and multiple electron numbers as well as satisfactory redox potential gap between the redox pair is essential to realizing high-performance *** molecular engineering,the redoxtargeting strategy is an effective way to obtain high-capacity *** further discuss and analyze the redox reaction mechanisms of organic redox species based on a series of electrochemical and spectroscopic approaches,and succinctly summarize the capacity degradation mechanisms of ***,the current challenges,opportunities,and future directions of organic redox-active materials for AORFBs are presented in detail.

关键词： aqueous redox flow batteries grid energy storage molecular engineering strategies organic redox-active materials redox reaction mechanisms

Pt-Ni nanourchins as electrocatalysts for oxygen reduction reaction

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Frontiers in Energy 2017年第3期11卷 254-259页

作者： Qiaowan CHANG Yuan XU Shangqian ZHU Fei XIAO minhua shao Department of Chemical and Biomolecular Engineering Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong China Department of Chemical and Biomolecular Engineering Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong China Energy Institute Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong China

Pt-Ni bimetallic alloys with various nanos-tructures have shown excellent activity toward oxygen reduction reaction （ORR）. The ORR activity is highly dependent on the structure of the catalyst. In this paper, Pt-Ni nanourchins were synthesized with an average size of 50 nm consisting of 10-20 nanorods and nanooctahedra by adjusting the synthesis condition. The formation of Pt-Ni nanourchins is mainly dependent on the adding order of solvents （benzyl ether, oleylamine and oleic acid）. Pt-Ni nanourchins present a reasonable high ORR activity （0.81 A/mg at 0.9 V）.

关键词： Pt-Ni alloys nanourchins oxygen reduction reaction shape control fuel cells

海胆状CoTe-CoP异质结构催化剂在全pH范围内高效析氢

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Science China Materials 2024年第6期67卷 1891-1899页

作者：朱少柯邢明辉路站宽乔泽龙王世涛赵青蓝邵敏华甑崇礼曹达鹏 State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Department of Chemical and Biological Engineering Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong 999077China Energy Institute and Chinese National Engineering Research Center for Control&Treatment of Heavy Metal PollutionThe Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong 999077China Qingdao International Academician Park Research Institute Qingdao 266000China School of Chemical Engineering The University of New South WalesSydney NSW 2052Australia

研发长效稳定、pH适应性强的析氢反应(HER)催化剂对实现大规模制氢具有重要意义.界面工程是研发高效HER催化剂的有效策略之一.本文成功构建了海胆状异质结构催化剂CoTe-CoP/***和CoP的协同作用不仅优化了电子结构、暴露了更多的活性位点... 详细信息

研发长效稳定、pH适应性强的析氢反应(HER)催化剂对实现大规模制氢具有重要意义.界面工程是研发高效HER催化剂的有效策略之一.本文成功构建了海胆状异质结构催化剂CoTe-CoP/***和CoP的协同作用不仅优化了电子结构、暴露了更多的活性位点,而且有效地提高了催化剂的亲水性和疏气性.密度泛函理论计算表明:CoTe与CoP之间的相互作用有效地降低了水的解离能垒,同时增强了对H~*的吸附.这些结果使得CoTe-CoP/NF在整个pH范围内具有优异的HER性能和催化稳定性.在酸性、碱性和中性介质中,CoTe-CoP/NF电极驱动10 mA cm^(-2)的电流密度仅需51、53和75 mV的过电位.总之,本工作为在全pH范围内构建高性能HER催化剂提供了一种界面工程新策略.

关键词： heterostructure hydrogen evolution reactions in-terface engineering all-pH range synergy effect

Superior oxygen electrocatalyst derived from metal organic coordination polymers by instantaneous nucleation and epitaxial growth for rechargeable Li-O_(2) battery

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Journal of Energy Chemistry 2023年第3期78卷 169-177,I0005页

作者： Dongdong Li Jinbiao Chen Yingtong Chen Yian Wang Yanpeng Fu minhua shao Zhicong Shi Institute of Batteries School of Materials and EnergyGuangdong University of TechnologyGuangzhou 510006GuangdongChina Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayKowloon 999077Hong KongChina Energy Institute The Hong Kong University of Science and TechnologyClear Water BayKowloon 999077Hong KongChina Guangzhou HKUST Fok Ying Tung Research Institute Guangzhou 511458GuangdongChina

Rechargeable aprotic Li-O_(2)batteries have attractea increasing attention due to their extremely high capacity,and it is very important to design appropriate strategies to synthesize efficient catalysts used as oxygen *** present work,we present an expedient "instantaneous nucleation and epitaxial growth"(INEG) synthesis strategy for convenient and large-scale synthesis of ultrafine MOCPs nanoparticles(size 50-100 nm) with obvious advantages such as fast synthesis,high yields,low costs and reduced synthetic *** bimetallic Ru/Co-MOCPs are further pyrolyzed to obtain bimetallic Coand low content of Ru-based nanoparticles embedded within nitrogen-doped carbon(Ru/Co@N-C) as an efficient catalyst used in Li-O_(2)*** Ru/Co@N-C provides porous carbon framework for the ion transportation and O_(2)diffusion,and has large amounts of metal/nonmetal sites as active site to promote the oxygen reduction reaction(ORR)/oxygen evolution reaction(OER) in Li-O_(2)*** a consequence,a high discharge specific capacity of 15246 mA h g^(-1)at 250 mA g^(-1), excellent rate capability at different current densities,and stable overpotential during cycling,are *** work opened up a new understanding for the industrialized synthesis of ultrafine catalysts for Li-O_(2)batteries with excellent structural characteristics and electrochemical performance.

关键词： Ultraﬁne MOCPs Expedient synthesis strategy Derivative Bimetallic sites Rechargeable Li-O_(2)batteries