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Tuning electronic structure of RuO_(2)by single atom Zn and oxygen vacancies to boost oxygen evolution reaction in acidic medium

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Journal of Energy Chemistry 2024年第1期88卷 94-102,I0003页

作者： Qing Qin Tiantian Wang Zijian Li Guolin Zhang Haeseong Jang Liqiang Hou Yu Wang Min Gyu Kim Shangguo liu xien liu College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Department of Chemistry City University of Hong KongHong Kong 999077China Department of Advanced Materials Engineering Chung-Ang UniversityAnseong-siGyeonggi-do 17546SeoulRepublic of Korea Beamline Research Division Pohang Accelerator Laboratory(PAL)Pohang 37673Gyeongsangbuk-doRepublic of Korea

The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.

关键词： Electrocatalyst Acidic oxygen evolution reaction Electronic structure engineering Durability Reaction barrier

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Electron-deficient ZnO induced by heterointerface engineering as the dominant active component to boost CO_(2)-to-formate conversion

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Carbon Energy 2024年第5期6卷 127-136页

作者： Qing Qin Zijian Li Yingzheng Zhang Haeseong Jang Li Zhai Liqiang Hou Xiaoqian Wei Zhe Wang Min Gyu Kim Shangguo liu xien liu College of Chemical Engineering Qingdao University of Science and TechnologyQingdaoChina Department of Chemistry City University of Hong KongHong Kong SARChina Department of Advanced Materials Engineering Chung-Ang UniversityAnseong-siGyeonggi-doRepublic of Korea Beamline Research Division Pohang Accelerator Laboratory(PAL)PohangRepublic of Korea

Electrocatalytic CO_(2)-to-formate conversion is considered an economically viable process.In general,Zn-based nanomaterials are well-known to be highly efficient electrocatalysts for the conversion of CO_(2) to CO,but seldom do they exhibit excellent selectivity toward formate.In this article,we demonstrate that a heterointerface catalyst ZnO/ZnSnO3 with nanosheet morphology shows enhanced selectivity with a maximum Faradaic efficiency(FE)of 86%at−0.9 V versus reversible hydrogen electrode and larger current density for the conversion of CO_(2) to formate than pristine ZnO and ZnSnO3.In particular,the FEs of the C1 products(CO+HCOO−)exceed 98%over the potential window.The experimental measurements combined with theoretical calculations revealed that the ZnO in ZnO/ZnSnO3 heterojunction delivers the valence electron depletion and accordingly optimizes Zn d-band center,which results in moderate Zn-O hybridization of HCOO*and weakened Zn-C hybridization of competing COOH*,thus greatly boosting the HCOOH generation.Our study highlights the importance of charge redistribution in catalysts on the selectivity of electrochemical CO_(2) reduction.

关键词： charge redistribution CO_(2)reduction reaction electrocatalyst heterointerfaces selectivity

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A survey of automated International Classification of Diseases coding:development,challenges,and applications

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Intelligent Medicine 2022年第3期2卷 161-173页

作者： Chenwei Yan Xiangling Fu xien liu Yuanqiu Zhang Yue Gao Ji Wu Qiang Li School of Computer Science Beijing University of Posts and TelecommunicationsBeijing 100876China Key Laboratory of Trustworthy Distributed Computing and Service(BUPT) Ministry of EducationBeijing 100876China Department of Electronic Engineering Tsinghua UniversityBeijing 100084China Beijing Tsinghua Changgung Hospital Beijing 102218China

The International Classification of Diseases(ICD)is an international standard and tool for epidemiological in-vestigation,health management,and clinical diagnosis with a fundamental role in intelligent medical care.The assignment of ICD codes to health-related documents has become a focus of academic research,and numerous studies have developed the process of ICD coding from manual to automated work.In this survey,we review the developmental history of this task in recent decades in depth,from the rules-based stage,through the traditional machine learning stage,to the neural-network-based stage.Various methods have been introduced to solve this problem by using different techniques,and we report a performance comparison of different methods on the pub-licly available Medical Information Mart for Intensive Care dataset.Next,we summarize four major challenges of this task:(1)the large label space,(2)the unbalanced label distribution,(3)the long text of documents,and(4)the interpretability of coding.Various solutions that have been proposed to solve these problems are analyzed.Further,we discuss the applications of ICD coding,from mortality statistics to payments based on disease-related groups and hospital performance management.In addition,we discuss different ways of considering and evaluat-ing this task,and how it has been transformed into a learnable problem.We also provide details of the commonly used datasets.Overall,this survey aims to provide a reference and possible prospective directions for follow-up research work.

关键词： International Classification of Diseases coding Disease classification Health-related document Electronic medical record Medical record management Clinical coding

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Oxygen-deficient SnO_(2)nanoparticles with ultrathin carbon shell for efficient electrocatalytic N_(2)reduction

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Green Energy & Environment 2022年第4期7卷 672-679页

作者： Guangkai Li Haeseong Jang Zijian Li Jia Wang Xuqiang Ji Min Gyu Kim xien liu Jaephil Cho State Key Laboratory Base of Eco-chemical Engineering College of Chemical EngineeringCollege of Chemistry and Molecular EngineeringQingdaoUniversity of Science and TechnologyQingdao266042China Department of Energy Engineering School of Energy and Chemical EngineeringUlsan National Institute of Science and Technology(UNIST)Ulsan689-798South Korea College of Materials Science and Engineering Qingdao UniversityQingdao266071China Beamline Research Division Pohang Accelerator Laboratory(PAL)Pohang790-784South Korea

For high-efficiency NH_(3)synthesis via ambient-condition electrohydrogenation of inert N_(2),it is pivotal to ingeniously design an active electrocatalyst with multiple features of abundant surfacial deficiency,good conductivity and large surface area.Here,oxygen-deficient SnO_(2)nanoparticles encapsulated by ultrathin carbon layer(d-SnO_(2)@C)are developed by hydrothermal deposition coupled with annealing process,as promising catalysts for ambient electrocatalytic N_(2)reduction.d-SnO_(2)@C exhibits high activity and excellent selectivity for electrocatalytic conversion of N_(2)to NH_(3)in acidic electrolytes,with Faradic efficiency as high as 12.7%at-0.15 V versus the reversible hydrogen electrode(RHE)and large NH_(3)yield rate of 16.68μg h^(-1)mgcat^(-1)at-0.25 V vs.RHE in 0.1 mol L^(-1)HCl.Benefiting from the structural superiority of enhanced charge transfer efficiency and optimized surface states,d-SnO_(2)@C also achieves excellent long-term stability.

关键词： N_(2)reduction reaction NH_(3)synthesis SnO_(2) Electrocatalysts Ambient conditions

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Ultrafine PdAg alloy nanoparticles anchored on NH2-functionalized 2D/2D TiO_(2) nanosheet/rGO composite as efficient and reusable catalyst for hydrogen release from additive-free formic acid at room temperature

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Journal of Energy Chemistry 2021年第8期30卷 455-464,I0010页

作者： Xi Zhao Ping Dai Dongyan Xu Xumei Tao xien liu Qingjie Ge State Key Laboratory Base of Eco-chemical Engineering College of Chemical EngineeringQingdao University of Science&TechnologyQingdao 266042China Shandong Provincial Key Laboratory Of Polymer Material Advanced Manufacturing Technology College of Electromechanical EngineeringQingdao University of Science&TechnologyQingdao 266061China Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering College of Chemistry and Chemical EngineeringNingxia University750021 YinchuanChina

A 2 D-2 D titanium dioxide nanosheet-reduced graphene oxide(TNS-r GO)composite with better electronic conductivity and hydrophilicity was prepared by the hydrothermal method.The as-obtained TNS-r GO composite was further functionalized with 3-aminopropyltriethoxysilane(APTES)to provide a large amount of-NH2 groups on the surface for anchoring ultrafine Pd Ag alloy nanoparticles with an average particle size of 1.69 nm by a facile wet reduction approach.Benefiting from the combined effects of well-dispersed Pd Ag alloy nanoparticles,facilitated electron transfer from TNS-r GO to Pd,and increased electron density of active sites,the Pd8 Ag_(1)/NH_(2)-TNS-r GO catalyst exhibited excellent activity towards dehydrogenation of formic acid without adding any additives at 298 K,corresponding to an initial turn over frequency as high as 1090 h-1,which is much higher than that of most other state-of-theart catalysts.

关键词： Formic acid Dehydrogenation TNS-rGO composite PdAg alloy Amine-functionalization

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Nitrogen, phosphorus co-doped carbon cloth as self-standing electrode for lithium-iodine batteries

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Nano Research 2019年第3期12卷 549-555页

作者： Kang Li Song Chen Si Chen xien liu Wei Pan Jintao Zhang Key Laboratory for Colloid and Interface Chemistry Ministry of Education School of Chemistry and Chemical Engineering Shandong University Jinan 250100 China State Key Laboratory Base of Eco-chemical Engineering College of Chemistry and Molecular Engineering Qingdao University of Science & Technology Qingdao 266042 China College of Chemistry Chemical Engineering and Materials Science Shandong Normal University Jinan 250014 China

Rechargeable lithium-iodine (Li-I2) battery is a promising energy storage system because of the high energy and power density. However, the shuttle effects of iodine species and the unstable features of l2 block the practical applications of Li-I2 batteries. Herein, a dual heteroatom doped porous carbon cloth is fabricated as the host material for lithium iodide (Lil). Specifically, the self-standing nitrogen, phosphorus co-doped carb on cloth with high Lil loading exhibits a large specific capacity (221 mAh·g^-1 at 1 C), excelle nt rate capability (95.8% capacity rete ntion at 5 C) and superior I ong cycli ng stability (2,000 cycles with a capacity rete ntion of 96%). Electrochemical kin etic an alysis con firms the domi nant contribution of capacitive effects at high sean rates, which is responsible for the good high-rate performance. The improved electrochemical performance mainly stems from two unique features of nitrogen, phosphorus co-doped porous carbon cloth. Heteroatom doping provides extra active sites for strong adsorption of iodine species while the highly porous structure with large surface area favors the capacitive effects at high rates. This work provides a facile yet efficient approach to regulating both redox reaction and capacitive effects via adjusting surface composition and pore structure of carbon materials for en hanced battery performance.

关键词： iodine heteroatom doping self-standing capacitive effect porous carbon

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Adsorption performance and physicochemical mechanism of MnO_(2)-polyethylenimine-tannic acid composites for the removal of Cu(Ⅱ) and Cr(Ⅵ) from aqueous solution

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Frontiers of Chemical Science and Engineering 2021年第3期15卷 538-551页

作者： Xiaoyan Deng Luxing Wang Qihui Xiu Ying Wang Hong Han Dongmei Dai Yongji Xu Hongtao Gao xien liu College of Environment and Safety Engineering State Key Laboratory Base of Eco-Chemical EngineeringQingdao University of Science&TechnologyQingdao 266042China College of Chemistry and Molecular Engineering State Key Laboratory Base of Eco-Chemical EngineeringQingdao University of Science&TechnologyQingdao 266042China

In this work,an adsorbent,which we call MnPT,was prepared by combining MnO_(2),polyethylenimine and tannic acid,and exhibited efficient performance for Cu(Ⅱ) and Cr(VI) removal from aqueous solution.The oxygen/nitrogen-containing functional groups on the surface of MnPT might increase the enrichment of metal ions by complexation.The maximum adsorption capacities of MnPT for Cu(Ⅱ) and Cr(Ⅵ) were 121.5 and 790.2 mg·g^(-1),respectively.The surface complexation formation model was used to elucidate the physicochemical interplay in the process of Cu(Ⅱ) and Cr(Ⅵ) co-adsorption on MnPT.Electrostatic force,solvation action,adsorbate-adsorbate lateral interaction,and complexation were involved in the spontaneous adsorption process.Physical electrostatic action was dominant in the initial stage,whereas chemical action was the driving force leading to adsorption equilibrium.It should be noted that after adsorption on the surface of MnPT,Cr(Ⅵ) reacted with some reducing functional groups(hydroxylamine-NH_(2))and was converted into Cr(Ⅲ).The adsorption capacity declined by 12% after recycling five times.Understanding the adsorption mechanism might provide a technical basis for the procedural design of heavy metal adsorbents.This MnPT nanocomposite has been proven to be a low-cost,efficient,and promising adsorbent for removing heavy metal ions from wastewater.

关键词： MnO_(2)-polyethylenimine-tannic acid composite surface complexation formation model Cu(Ⅱ) Cr(Ⅵ) physicochemical mechanism

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磷掺杂碳负载Zn_(x)P_(y)O_(z)常温常压下高效电催化合成氨

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物理化学学报 2024年第3期40卷 29-30页

作者：王佳秦清王哲赵旭浩陈云菲候利强刘尚果刘希恩青岛科技大学化工学院山东青岛266042

合成氨(NH_(3))的发展是现代工业进程和人类生存的基石。受氮气(N_(2))化学惰性的限制,当前的合成氨工业能源消耗高并且排放大量的二氧化碳。电化学氮气还原反应(NRR),是有望取代高能耗的Haber-Bosch(HB)合成法的一种绿色可持续的合成... 详细信息

合成氨(NH_(3))的发展是现代工业进程和人类生存的基石。受氮气(N_(2))化学惰性的限制,当前的合成氨工业能源消耗高并且排放大量的二氧化碳。电化学氮气还原反应(NRR),是有望取代高能耗的Haber-Bosch(HB)合成法的一种绿色可持续的合成氨工艺。然而,因氮气以及析氢竞争富反应(HER)导致电催化氮气还原极低的NH_(3)产率和能量转换效率一直是目前人工固氮领域面临的挑战。在本文中,我们报道了一种具有丰富孔结构的磷掺杂碳(PC)负载Zn_(3)(PO_(4))_(2)/Zn_(2)P_(2)O_(7)纳米复合材料(h-PC/Zn_(3)(PO_(4))_(2)/Zn_(2)P_(2)O_(7)),在酸性和中性介质中将N_(2)高效催化转化为NH_(3)。其独特的分级多孔结构提高了表面粗糙度并加快了氮气在催化剂体相中的扩散,这有利于延长氮气在催化剂表面的停留时间以及提高活性位点的利用效率。而多组分的均匀分布可以调节电子结构并优化反应中间体的吸附行为,进而提高活性位点的本征活性。在0.1mol·L^(-1)HCI电解液中,h-PC/Zn_(3)(PO_(4))_(2)/Zn_(2)P_(2)O_(7)在-0.2 V vs.可逆氢电极(RHE)电位下NH_(3)的产率可以达到38.7±1.2μg·h^(-1)·mgcat^(-1),法拉第效率为19.8%±0.9%。此外;h-PC/Zn_(3)(PO_(4))_(2)/Zn_(2)P_(2)O_(7)在0.1 mol·L^(-1)Na_(2)SO_(4)溶液中同样展现出优异的电催化氮气还原合成氨性能,NH_(3)产率及法拉第效率分别为17.1±0.8μg·h^(-1)·mgcat^(-1)和15.g%±0.6%,明显优于PC/Zn_(3)P_(2)、C/ZnO和大多数报道的非贵金属电催化剂。这种优异的性能主要归因于多孔结构有利于传质及多组分活性位点协同效应。此外,我们采用非原位X射线光电子能谱(XPS)、透射电子显微镜(TEM)和X射线衍射(XRD)等表征手段对NRR测试前后h-PC/Zn_(3)(PO_(4))_(2)/Zn_(2)P_(2)O_(7)的组成和结构变化进行了剖析。在反应后检测到了新增的N物种信号,证明催化剂确实发生了氮气还原反应。本研究提供了一种通过同步构建传质通道并耦合不同的活性位点以协同增强NRR活性和选择性的新思路,这对加快绿色制氨工业化具有重大意义。

关键词：氮气还原反应电催化剂孔结构多活性中心协同效应

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大语言模型基本医学能力及其在脑血管病等临床应用上的研究进展

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中国卒中杂志 2024年第6期19卷 613-620页

作者：刘喜恩刘少辉周开银尤心心周宇轩宁辰傅湘玲吴及清华大学电子工程系北京100084 北京邮电大学计算机学院北京惠及智医科技有限公司清华大学人工智能学院

近年来,大语言模型在通用领域涌现出了惊人的智慧能力,并快速在各行业得到了广泛而有效的应用。然而,临床医学领域由于专业性强、场景复杂,大语言模型能否提供准确、可靠、高效的医疗服务,目前还没有形成一致性的结论。本研究从以下几... 详细信息

近年来,大语言模型在通用领域涌现出了惊人的智慧能力,并快速在各行业得到了广泛而有效的应用。然而,临床医学领域由于专业性强、场景复杂,大语言模型能否提供准确、可靠、高效的医疗服务,目前还没有形成一致性的结论。本研究从以下几个方面对大语言模型在临床医学中的研究进展进行综述:医学知识和基本医学能力评测情况;临床场景特定能力方面的研究进展;脑血管病等临床疾病及相关临床应用方面的研究进展。

关键词：大语言模型医疗大语言模型智慧医疗

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随钻中继式电磁波传输技术及应用研究

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电声技术 2024年第1期48卷 90-94页

作者：赵龙刘西恩孙向阳张利伟中海油田服务股份有限公司北京110049 电子科技大学四川成都611731

针对随钻条件下无线电磁波传输技术信号衰减大、传播距离短、信号频率低以及传输速率慢的难题,文章设计了基于准横电磁波(Transverse Electromagnetic Wave,TEM)激励模式的随钻中继式电磁波传输技术。该技术以钻杆作为传输载体,将电磁... 详细信息

针对随钻条件下无线电磁波传输技术信号衰减大、传播距离短、信号频率低以及传输速率慢的难题,文章设计了基于准横电磁波(Transverse Electromagnetic Wave,TEM)激励模式的随钻中继式电磁波传输技术。该技术以钻杆作为传输载体,将电磁波在井内的随钻传输模型类比同轴线传输模型,通过使用多组载波频率,在提高传输速率的同时,利用中继接力扩展传输距离。该技术已通过不同地层环境的现场验证,是井下数据传输未来发展的重要方向。

关键词：随钻测井电磁传输中继式

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