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Single-atom catalysts with anionic metal centers: Promising electrocatalysts for the oxygen reduction reaction and beyond

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Journal of Energy Chemistry 2021年第12期30卷 285-293,I0006页

作者： Jinxing gu Yinghe Zhao Shiru Lin Jingsong Huang Carlos R.Cabrera Bobby G.Sumpter Zhongfang Chen Department of Chemistry University of Puerto Rico.Rio Piedras Campus.San Juan.Puerto Rico 00931USA Center for Nanophase Materials Sciences Oak Ridge National LaboratoryOak RidgeTennessee 37831USA Department of Chemistry and Biochemistry The University of Texas at El PasoEl PasoTexas 79968USA

Ongoing efforts to develop single-atom catalysts(SACs) for the oxygen reduction reaction(ORR) typically focus on SACs with cationic metal centers,while SACs with anionic metal centers(anionic SACs) have been generally ***,anionic SACs may offer excellent active sites for ORR,since anionic metal centers could facilitate the activation of O_(2) by back donating electrons to the antibonding orbitals of O_(2).In this work,we propose a simple guideline for designing anionic SACs:the metal centers should have larger electronegativity than the surrounding atoms in the substrate on which the metal atoms are *** means of density functional theory(DFT) simulations,we identified 13 anionic metal centers(Co,Ni,Cu,Ru,Rh,Pd,Ag,Re,Os,Ir,Pt,Au,and Hg) dispersed on pristine or defective antimonene substrates as new anionic SACs,among which anionic Au and Co metal centers exhibit limiting potentials comparable to,or even better than,conventional Pt-based catalysts towards *** also found that anionic Os and Re metal centers on the defective antimonene can electrochemically catalyze the nitrogen reduction reaction(NRR) with a limiting potential close to that of stepped Ru(0001).Overall,our work shows promise towards the rational design of anionic SACs and their utility for applications as electrocatalysts for ORR and other important electrochemical reactions.

关键词： Single-atom catalysts Anionic metal centers Antimonene Oxygen reduction reaction Nitrogen reduction reaction

Single thiolate replacement of metal nanoclusters

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Science China Chemistry 2024年第2期67卷 523-528页

作者： Ambreen Ambreen Yue Zhou Wanmiao gu Qing You Liang Fang guoqing Bian Nan Yan Nan Xia zhikun Wu Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and NanotechnologyInstitute of Solid State PhysicsHefei Institutes of Physical Science(HFIPS)Chinese Academy of SciencesHefei230031China University of Science and Technology of China Hefei230601China Institute of Physical Science and Information Technology Anhui UniversityHefei230601China

Surface thiolates play important roles in evincing the structures and properties of thiolated metal nanoclusters—one type of recently emerging inorganic-organic hybrids,and thus the thiolate substitution,especially single thiolate substitution,is highly desirable for subtly tailoring the structures and properties of metal ***,such a single-thiolate substituting is challenging,and its influence on the metal-metal and metal-sulfur bonds remains mysterious due to the absence of the singlethiolate-substituted ***,we developed a combined method,concurrently synthesized the single-thiolate-substituted nanocluster and its parent nanocluster,and successfully resolved their structures by single crystal X-ray crystallography,which reveals that the single thiolate substitute has an obvious influence on the metal-metal and metal-sulfur bond lengths although it has no effect on the absorption ***,the metal-metal and metal-sulfur bonds show various thermal extensibility and even the negative thermal expansion phenomena of the Au–S bond were observed in the single-thiolate-substituted *** bond length-related stability was also ***,this study highlights a novel synthesis method and offers novel structural insights and an in-depth structure-property correlation of thiolated metal nanoclusters.

关键词： metal nanoclusters single thiolate replacement thermal expansion stability intercluster interaction

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电磁轨道发射装置反后坐技术研究

南京理工大学学报 2020年第6期44卷 759-764页

作者：古刚宋海通马新科海军工程大学舰船综合电力技术国防科技重点实验室湖北武汉430033 中国船舶重工集团公司第七一三研究所河南郑州450015

电磁轨道发射装置在发射过程中存在后坐力,为研究其反后坐技术,该文结合某电磁轨道发射装置模型,建立了后坐运动微分方程,设计了两种反后坐装置方案,进行了发射装置在0°、35°和70°3种射角工况下分别采用两种反后坐装置方案时的后坐... 详细信息

电磁轨道发射装置在发射过程中存在后坐力,为研究其反后坐技术,该文结合某电磁轨道发射装置模型,建立了后坐运动微分方程,设计了两种反后坐装置方案,进行了发射装置在0°、35°和70°3种射角工况下分别采用两种反后坐装置方案时的后坐规律仿真计算,试验验证了仿真计算模型有效。对仿真计算结果进行对比分析,得出结论:对于具有大后坐部分质量和宽射角范围的电磁轨道发射装置,采用2套复进机和2套驻退机分别对称布置在身管的上下和左右两侧的反后坐装置方案,能够有效提高反后坐装置密封可靠性,避免后坐部分受到偏转力矩作用。

关键词：兵器科学与技术电磁轨道发射装置后坐力后坐规律运动仿真

Pollen-like self-supported FeIr alloy for improved hydrogen evolution reaction in acid electrolyte

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Journal of Energy Chemistry 2022年第3期31卷 560-565,I0015页

作者： Shengyu Ma Jun Deng Yaping Xu Weiying Tao Xiaoqi Wang zhiping Lin Qinghua Zhang Lin gu Wenwu Zhong School of Advanced Study Taizhou UniversityTaizhou 318000ZhejiangChina Taizhou Research Institute of Bio-medical and Chemical Industry CO. LTDTaizhou 318000ZhejiangChina Institution of Physics Chinese Academic of ScienceBeijing 100190China

Ir is recognized as efficient catalyst for hydrogen evolution reaction(HER).The high price,however,has hindered its application in the production of *** this work,we prepared the self-supported FeIr alloy nanoparticles,taking advantage of solid-state synthesis *** as-prepared FeIr alloy possesses a novel morphology of pollen,which is consist of smaller FeIr *** calculations reveal that the change of the free Gibbs for Ir is negative after the adsorption of active H,while it is positive for the case of ***,the alloying of Fe and Ir not only effectively reduces the cost,but also can achieve more adequate adsorption of active H *** from this,the as-prepared FeIr alloy nanoparticle exhibits superior HER performance with an overpotential of 19 m V at a current density of 10 m V/cm^(2)and a Tafel slope of 32 m V/dec,when tested in 0.5 M H_(2)SO_(4),better than pure Ir and Pt/*** work paves the way to the exploration of efficient alloy electrocatalysts for HER.

关键词： FeIr alloy Water splitting Catalysis Hydrogen evolution reaction

Sierpiński triangles formed by molecules with linear backbones on Au(111)

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Chinese Chemical Letters 2018年第6期29卷 967-969页

作者： Xue Zhang Ruoning Li Na Li Gaochen gu Yajie Zhang Shimin Hou Yongfeng Wang Key laboratory for the Physics and Chemistry of Nanodevices Department of Electronics Peking University Beijing 100871 China Peking University Information Technology Institute Tianjin Tianjai Tianjin 300450 China

Fractals play an important role in mathematics, aesthetic, science, and engineering. The representative Sierpinski-triangle fractals have been successfully constructed by V-shape molecules in experiments. The molecular Sierpinski triangles formed by molecules with linear backbones have been theoretically predicted but not experimentally discovered. To achieve this goal in the experiment, we used[1,1’;4’,1’’;4’’,1’’’]-quaterphenyl-3,40 0-dicarbonitrile molecules as building blocks and employed cobalt atoms as cements, then successfully obtained metal-organic Sierpinski triangles with an order up to 2 on the Au（111） surface. There are twenty-four types of three-fold coordination nodes formed between the metal atom and organic ligands via coordinate interactions. The coexistence of various nodes is responsible for that the highest order of Sierpinski triangles is limited to 2.

关键词： STM linear backbone Coordination Fractal Sierpinski triangle

Comparison of brain functions between healthy participants and methamphetamine users with various addiction histories:Data analysis based on EEG and fNIRS

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Journal of Innovative Optical Health Sciences 2024年第3期17卷 41-55页

作者： Xuelin gu Xiaoou Li Banghua Yang College of Medical Instruments Shanghai University of Medicine&Health SciencesShanghai 201318P.R.China School of Mechanical and Electrical Engineering and Automation Shanghai UniversityShanghai 200444P.R.China

The electroencephalogram(EEG)rhythm and functional near-infrared spectroscopy(fNIRS)activation levels have not been compared between a healthy control group(HCG)and methamphetamine user group(MUG)with different addiction *** study used 64-electrode EEG and fNIRS to conduct an experiment that analyzed the resting and craving *** EEG and fNIRS data of 56 participants were collected,including 14 healthy participants,14 methamphetamine users with an addiction history of 0.5–5 years,14 users with an addiction history of 5–10 years,and 14 users with an addiction history of 10–15 *** effective coherence(iCoh)within the brain network was used to process the EEG *** analysis was performed to compare differences in iCoh among the delta,theta,alpha,beta,and gamma bands and explore oxyhemoglobin activation levels in the ventrolateral prefrontal cortex,dorsolateral prefrontal cortex,orbitofrontal cortex,and frontopolar prefrontal cortex(FPC)of the control ***,the Kmeans,Gaussian mixed model(GMM),linear discriminant analysis(LDA),support vector machine(SVM),Bayes,and convolutional neural networks(CNN)algorithms were used to classify methamphetamine users based on drug and neutral images.A 3-class accuracy was *** in EEG and fNIRS activation levels of HCG and MUG with varied addiction histories were demonstrated.

关键词： Drug addiction history electroencephalogram functional near-infrared spectroscopy isolated effective coherence addiction history classification

Effect of three insect-resistant maizes expressing Cry1le,Cry1Ab/Cry2Aj and Cry1Ab on the growth and development of armyworm Mythimna separata(Walker)

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Journal of Integrative Agriculture 2020年第7期19卷 1842-1849页

作者： SU Hong-hua JIANG Tao SUN Yu gu Hui-jie WU Jiao-jiao YANG Yi-zhong School of Horticulture and Plant Protection Yangzhou UniversityYangzhou 225009P.R.China

Three transgenic maize events(IE09S034,Shuangkang 12--5 and C0030.3.5)produced Cry1le,Cry1Ab/Cry2Aj and G10-EPSPS,Cry1Ab and EPSPS,respectively,all of which target the Asian corn *** oriental armyworm Mythimna separata(Walker)is the secondary *** this study,the effects of the three Bt maizes on the development and survival of armyworm were *** results showed that IE09S034 had insecticidal activity against 1st instar larvae,and the survival rate of armyworm fed with Bt maize for 10 days was 462%,significantly lower than that of the *** larvae at 3rd--6th instar were more tolerant of the Bt toxin than the early instar ***,Shuangkang 12-5 had good insecticidal activity against 1st-5th instar *** mortality was nearly 100%when the larvae were fed with Shuangkang 12-5 before 3rd instar,and the toxin had quick acting *** event significantly ihibited the development of armyworm;that is,the larval duration of the 3rd and 4th instar larvae fed with Shuangkang 12-5 was prolonged by 4.5 and 3.0 days,*** pupal weight and egg number were also significantly lower than those of the *** C0030.3.5,it could control 1st--5th instar larvae *** mortality rates were all over 50%if 1st-3rd larvae were fed with this *** pupal weight of 4th-6th instar larvae fed with Bt maize were only 53.9,56.8 and 54.6%,respectively,compared to that of the *** number of eggs laid was significantly less than the *** results indicate that all three transgenic maize events exhibit the potential to provide effective control of early instar larvae of *** can be commercialized in future to control lepidoptera pests such as Asian corn borer and armyworm.

关键词： transgenic maize armyworm development survival

A facile path from fast synthesis of Li-argyrodite conductor to dry forming ultrathin electrolyte membrane for high-energy-density allsolid-state lithium batteries

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Journal of Energy Chemistry 2022年第11期31卷 309-316,I0008页

作者： Zhao Jiang Hongling Peng Jingru Li Yu Liu Yu Zhong Changdong gu Xiuli Wang Xinhui Xia Jiangping Tu State Key Laboratory of Silicon Materials Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Provinceand School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina CCTEG Chongqing Research Institute Chongqing 400039China

All-solid-state lithium batteries(ASSLBs),utilizing sulfide solid electrolyte,are considered as the promising design on account of their superior safety and high energy density,whereas the time-consuming preparation process of sulfide electrolyte powders and the thickness of electrolyte layer hinder their practical ***,an innovative ultimate-energy mechanical alloying plus rapid thermal processing approach is employed to rapidly synthesize the crystalline Argyrodite-type conductor Li_(5.3)PS_(4.3)ClBr_(0.7)(LPSCIBr)with superior ionic conductivity(11.7 mS cm^(-1)).Furthermore,to realize the higher energy density of the battery,an ultrathin LPSCIBr sulfide electrolyte membrane with superior ionic conductivity of 6.5 mS cm^(-1)is fabricated with the aid of polytetrafluoroethylene(PTFE)binder and the reinforced cellulose ***,a simple solid electrolyte interphase(SEI)is constructed on the surface of lithium metal to enhance anodic *** from the joint efforts of these merits,the modified ASSLBs with a high cell-level energy density of 311 Wh kg^(-1) show an excellent cyclic *** assembled all-solid-state Li_(2) S/Li pouch cell can operate even under the severe conditions of bending and cutting,demonstrating the enormous potential of the sulfide electrolyte membrane for ASSLBs application.

关键词： Sulfide electrolyte Thermal processing Ultrathin membrane Ionic conductivity All-solid-state lithium battery

黏弹性地基中基坑开挖对邻近桩基变形影响的时域解

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岩土力学 2017年第10期38卷 3017-3028,3038页

作者：张治国鲁明浩宫剑飞上海理工大学环境与建筑学院上海200093 国土资源部丘陵山地地质灾害防治重点实验室福建福州350002 中国建筑科学研究院建筑安全与环境国家重点实验室北京100013

目前就软土基坑开挖卸荷对邻近桩基变形影响的研究一般是基于瞬时开挖工况,很少考虑时间效应对桩-土相互作用的影响,但实际工程中软土在开挖情况下具有较为明显的流变效应。从地基黏弹性角度出发,采用两阶段法研究了黏弹性地基中基坑开... 详细信息

目前就软土基坑开挖卸荷对邻近桩基变形影响的研究一般是基于瞬时开挖工况,很少考虑时间效应对桩-土相互作用的影响,但实际工程中软土在开挖情况下具有较为明显的流变效应。从地基黏弹性角度出发,采用两阶段法研究了黏弹性地基中基坑开挖与邻近桩基相互作用的时域问题。第1阶段基于Boltzmann黏弹性模型推导出Mindlin时域解,用于分析黏弹性地基中基坑开挖引起的邻近桩基处的土体附加应力;第2阶段采用Pasternak地基模型分析桩基与黏弹性土体之间的相互作用,并求得考虑流变效应的桩基水平变形的简化时域解。最后,采用大型有限差分软件对相关工况进行数值模拟,并将数值模拟结果与简化时域解进行对比分析,得到了较好的一致性。此外,也针对Boltzmann黏弹性模型参数(体积模量、剪切模量、黏性系数)、桩径、基坑开挖深度、桩与基坑间距和基坑开挖尺寸进行了影响因素分析。分析结果表明,所得出的简化时域解能较好地反映基坑开挖对邻近桩基水平变形的影响,以及桩基变形随时间的发展趋势,可为相关实际工程提供一定理论依据。

关键词：基坑工程桩基黏弹性 Boltzmann模型时域分析