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Surface engineering of 1D nanocatalysts for value-added selective electrooxidation of organic chemicals

Nano Research 2024年第3期17卷 1327-1336页

作者： Yongping Yang Chuhao Liu Tinglu Song Mufan Li zipeng zhao Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications Experimental Center of Advanced MaterialsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Electrolytic water splitting by renewable energy is a technology with great potential for producing hydrogen(H_(2))without carbon emission,but this technical route is hindered by its huge energy(electricity)cost,which is mainly wasted by the anode oxygen evolution reaction(OER)while the value of the anode product(oxygen)is very limited.Replacing the high-energy-cost OER with a selective organic compound electrooxidation carried out at a relatively lower potential can reduce the electricity cost while producing value-added chemicals.Currently,H_(2) generation coupled with synthesis of value-added organic compounds faces the challenge of low selectivity and slow generation rate of the anodic products.One-dimensional(1D)nanocatalysts with a unique morphology,well-defined active sites,and good electron conductivity have shown excellent performance in many electrocatalytic reactions.The rational design and regulation of 1D nanocatalysts through surface engineering can optimize the adsorption energy of intermediate molecules and improve the selectivity of organic electrooxidation reactions.Herein,we summarized the recent research progress of 1D nanocatalysts applied in different organic electrooxidation reactions and introduced several different fabrication strategies for surface engineering of 1D nanocatalysts.Then,we focused on the relationship between surface engineering and the selectivity of organic electrooxidation reaction products.Finally,future challenges and development prospects of 1D nanocatalysts in the coupled system consisting of organic electrooxidation and hydrogen evolution reactions are briefly outlined.

关键词： hydrogen generation organic compound electrooxidation one-dimensional(1D)nanocatalysts surface engineering selectivity

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Stability of dimensionally stable anode for chlorine evolution reaction

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Nano Research 2024年第3期17卷 949-959页

作者： Ziliang Deng Shuying Xu Chuhao Liu Xueqiang Zhang Mufan Li zipeng zhao Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications Experimental Center of Advanced MaterialsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Laser Micro/Nano-Fabrication Laboratory School of Mechanical EngineeringBeijing Institute of TechnologyBeijing 10081China

Chlorine(Cl2)is one of the most important chemicals produced by the electrolysis of brine solutions and is a key raw material for many areas of industrial chemistry.For nearly half a century,dimensionally stable anode(DSA)made from a mixture of RuO_(2) and TiO_(2) solid oxides coated on Ti substrate has been the most widely used electrode for chlorine evolution reaction(CER).In harsh operating environments,the stability of DSAs remains a major challenge greatly affecting their lifetime.The deactivation of DSAs significantly increases the cost of the chlor-alkali industry due to the corrosion of Ru and the formation of the passivation layer TiO_(2).Therefore,it is urgent to develop catalysts with higher activity and stability,which requires a thorough understanding of the deactivation mechanism of DSA catalysts.This paper reviews existing references on the deactivation mechanisms of DSA catalysts,including both experimental and theoretical studies.Studies on how CER selectivity affects electrode stability are also discussed.Furthermore,studies on the effects of the preparation process,elemental composition,and surface/interface structures on the DSA stability and corresponding improvement strategies are summarized.The development of other non-DSA-type catalysts with comparable stability is also reviewed,and future opportunities in this exciting field are also outlined.

关键词： chlorine evolution reaction(CER) dimensionally stable anode(DSA) RuO_(2)-TiO_(2) metal oxide anode stability

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The Active Sites and Corresponding Stability Challenges of the M-N-C Catalysts for Proton Exchange Membrane Fuel Cell

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Chinese Journal of Chemistry 2023年第6期41卷 710-724页

作者： Ruolin Peng Zhongkun zhao Hongmin Sun Yongping Yang Tinglu Song Yao Yang Jiankun Shao Haibo Jin Hongtao Sun zipeng zhao Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications Experimental Center of Advanced MaterialsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing100081China The Harold and Inge Marcus Department of Industrial and Manufacturing Engineering The Pennsylvania State UniversityUniversity ParkPA16802-4400USA School of Engineering Westlake UniversityHangzhouZhejiang 310030China State Key Laboratory of Explosion Science and Technology Bejing Institute of TechnologyBeijing 100081China The Materials Research institute The Pennsylvania State UniversityUniversityParkPA16802-4400UA

Proton exchange membrane fuel cells(PEMFCs)as promising alternatives to traditional internal combustion engines have attracted massive concerns to promote their wide application in society.However,the biggest challenge to the commercialization of PEMFCs remains the high cost due to the adoption of the platinum group metal(PGM)catalysts in the cathode.

关键词： Proton exchange membrane fuel cell Electrocatalysis Oxygen reduction reaction M-N-C catalysts Active sites Stability Degradation mechanisms

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美国网络联盟体系的系统效应分析

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国家安全论坛 2024年第2期 40-49,87页

作者：赵子鹏国防大学国家安全学院

维护网络安全既是美国组建网络联盟的重要旗号,更是诸多国家加入这一联盟的首要诉求。但是,美国对网络议题的泛安全化策略,导致其主导下的网络联盟无论是成员组成还是层级结构,均进入持续扩张状态。目前,美国网络联盟已经从以美国为单... 详细信息

维护网络安全既是美国组建网络联盟的重要旗号,更是诸多国家加入这一联盟的首要诉求。但是,美国对网络议题的泛安全化策略,导致其主导下的网络联盟无论是成员组成还是层级结构,均进入持续扩张状态。目前,美国网络联盟已经从以美国为单一核心、重点聚焦网络空间军事议题的简单结构,扩张为一种复杂结构联盟体系,即联盟内不同成员国围绕不同议题动态组合小圈子,同时衍生出多个在美国之下、与美国有所争权的“二级核心”。复杂性科学指出,任何系统都面临“结果不随意图而来”的系统效应。在美国网络联盟体系中,这类系统效应表现为联盟体系具有将局部冲突扩大化的倾向、更多国家入盟后的集体行动能力不增反降、网络安全的重大威胁有时源自联盟内部、系统外部因素的快速进化削弱联盟内部控制力等,从而导致其结果更具不确定性。

关键词：网络安全网络联盟泛安全化系统效应

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Synthesis of surface controlled nickel/palladium hydride nanodendrites with high performance in benzyl alcohol oxidation

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Nano Research 2019年第6期12卷 1467-1472页

作者： zipeng zhao Michelle M.Flores Espinosa Jihan Zhou Wang Xue Xiangfeng Duan Jianwei Miao Yu Huang Department of Materials Science and Engineering University of CaliforniaLos AngelesCA 90095USA Department of Physics and Astronomy University of CaliforniaLos AngelesCA 90095USA Department of Chemistry and Biochemistry University of CaliforniaLos AngelesCA 90095USA California Nanosystems Institute University of CaliforniaLos AngelesCA 90095USA

Benzaldehyde byproduct is an imperative intermediate in the production of fine chemicals and additives.Tuning selectivity to benzaldehyde is therefore critical in alcohol oxidation reactions at the industrial level.Herein,we report a simple but innovative method for the synthesis of palladium hydride and nickel palladium hydride nanodendrites with controllable morphology,high stability,and excellent catalytic activity.The synthesized dendrites can maintain the palladium hydride phase even after their use in the chosen catalytic reaction.Remarkably,the high surface area morphology and unique interaction between nickel-rich surface and palladium hydride (β-phase) of these nanodendrites are translated in an enhanced catalytic activity for benzyl alcohol oxidation reaction.Our Ni/PdH0.43 nanodendrites demonstrated a high selectivity towards benzaldehyde of about 92.0% with a conversion rate of 95.4%,showing higher catalytic selectivity than their PdH0.43 counterparts and commercial Pd/C.The present study opens the door for further exploration of metal/metal-hydride nanostructures as next-generation catalytic materials.

关键词： benzyl alcohol selectivity benzaldehyde palladium hydride oxidation nanodendrites

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Pt3Ag alloy wavy nanowires as highly effective electrocatalysts for ethanol oxidation reaction

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Nano Research 2020年第5期13卷 1472-1478页

作者： Xiaoyang Fu Chengzhang Wan Aixin Zhang zipeng zhao Huaixun Huyan Xiaoqing Pan Shuaijing Du Xiangfeng Duan Yu Huang Department of Chemistry and Biochemistry University of CaliforniaLos AngelesLos AngelesCalifornia 90095USA Department of Materials Science and Engineering University of CaliforniaLos AngelesLos AngelesCalifornia 90095USA Department of Chemical Engineering and Materials Science University of CaliforniaIrvineIrvineCalifornia 92697USA Irvine Materials Research Institute(IMRI) University of CaliforniaIrvineIrvineCalifornia 92697USA Department of Physics and Astronomy University of CaliforniaIrvineIrvineCalifornia 92697USA California Nanosystems Institute University of CaliforniaLos AngelesLos AngelesCalifornia 90095USA

Direct ethanol fuel cell(DEFC)has received tremendous research interests because of the more convenient storage and transportation of ethanol vs.compressed hydrogen.However,the electrocatalytic ethanol oxidation reaction typically requires precious metal catalysts and is plagued with relatively high over potential and low mass activity.Here we report the synthesis of Pt3Ag alloy wavy nanowires via a particle attachment mechanism in a facile solvothermal process.Transmission microscopy studies and elemental analyses show highly wavy nanowire structures with an average diameter of 4.6±1.0 nm and uniform Pt3Ag alloy formation.Electrocatalytic studies demonstrate that the resulting alloy nanowires can function as highly effective electrocatalysts for ethanol oxidation reactions(EOR)with ultrahigh specific activity of 28.0 mA/cm^2 and mass activity of 6.1 A/mg,far exceeding that of the commercial Pt/carbon samples(1.10 A/mg).The improved electrocatalytic activity may be partly attributed to partial electron transfer from Ag to Pt in the Pt3Ag alloy,which weakens CO binding and the CO poisoning effect.The one-dimensional nanowire morphology also contributes to favorable charge transport properties that are critical for extracting charge from catalytic active sites to external circuits.The chronoamperometry studies demonstrate considerably improved stability for long term operation compared with the commercial Pt/C samples,making the Pt3Ag wavy nanowires an attractive electrocatalyst for EOR.

关键词： platinum silver alloy wavy nanowires electrocatalysis ethanol oxidation reaction(EOR)

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In situ development of highly concave and compositionconfined PtNi octahedra with high oxygen reduction reaction activity and durability

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Nano Research 2016年第1期9卷 149-157页

作者： Enbo Zhu Yongjia Li Chin-Yi Chiu Xiaoqing Huang Mufan Li zipeng zhao Yuan Liu Xiangfeng Duan Yu Huang Department of Materials Science and Engineering University of California Los Angeles CA 90095 USA Department of Chemistry and Biochemistry University of California Los Angeles CA 90095 USA California NanoSystems Institute University of California Los Angeles CA 90095 USA

Controlled syntheses of PtNi metal nanocrystals with unique structures for catalyzing oxygen reduction reactions （ORRs） have attracted great interest. Here, we report the one-step synthesis of single-crystal PtNi octahedra with in situ-developed highly concave features and self-confined composition that are optimal for ORR. Detailed studies revealed that the Pt-rich seeding, subsequent Pt/Ni co-reduction, and Pt-Ni interfusion resulted in uniform single-crystal PtNi octahedra, and that the combination of Ni facet segregation and oxygen etching of a Ni-rich surface led to the concavity and confined Ni content. The concave PtNi nanocrystals exhibited much higher ORR performance than the commercially available Pt/C catalyst in terms of both specific activity （29.1 times higher） and mass activity （12.9 times higher） at 0.9 V （vs. reversible hydrogen electrode （RHE））. The performance was also higher than that of PtNi octahedra without concavity, confirming that the higher activity was closely related to its morphology. Moreover, the concave octahedra also exhibited remarkable stability in ORR （93% mass activity remained after 10,000 cycles between 0.6 and 1.1 V vs. RHE） owing to the passivation of the unstable sites.

关键词： PtNi alloy,concave,oxygen reduction reaction

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Ultrathin wavy Rh nanowires as highly effective electrocatalysts for methanol oxidation reaction with ultrahigh ECSA

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Nano Research 2019年第1期12卷 211-215页

作者： Xiaoyang Fu zipeng zhao Chengzhang Wan Yiliu Wang Zheng Fan Frank Song Bocheng Cao Mufan Li Wang Xue Yu Huang Xiangfeng Duan Department of Chemistry and Biochemistry University of CaliforniaLos AngelesLos AngelesCalifornia 90095USA Department of Materials Science and Engineering University of CaliforniaLos AngelesLos AngelesCalifornia 90095USA California Nanosystems Institute University of CaliforniaLos AngelesLos AngelesCalifornia 90095USA

Direct methanol fuel cells (DMFCs) have received tremendous research interests because of the facile storage of liquid methanol vs.hydrogen.However,the DMFC today is severely plagued by the poor kinetics and rather high overpotential in methanol oxidation reaction (MOR).Here we report the investigation of the ultrathin Rh wavy nanowires as a highly effective MOR electrocatalyst.We show that ultrathin wavy Rh nanowires can be robustly synthesized with 2-3 nm diameters.Electrochemical studies show a current peak at the potential of 0.61 V vs.reversible hydrogen electrode (RHE),considerably lower than that of Pt based catalysts (~ 0.8-0.9 V vs.RHE).Importantly,with ultrathin diameters and favorable charge transport,the Rh nanowires catalysts exhibit an ultrahigh electrochemically active surface area determined from CO-stripping (ECSAco) of 144.2 m2/g,far exceeding that of the commercial Rh black samples (20 m2/g).Together,the Rh nanowire catalysts deliver a mass activity of 722 mA/mg at 0.61 V,considerably higher than many previously reported electrocatalysts at the same potential.The chronoamperometry studies also demonstrate good stability and CO-tolerance compared with the Rh black control sample,making ultrathin Rh wavy nanowires an attractive electrocatalyst for MOR.

关键词： rhodium nanowires electrocatalysis methanol oxidation reaction (MOR)

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基于ARIMA模型对定西天气数据的分析与预测

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现代信息科技 2024年第9期8卷 140-143页

作者：赵子鹏魏新奇唐龙高丙翻康亮河甘肃农业大学甘肃兰州730070

由于天气对农业生产、水资源管理和自然灾害预防等具有重要影响,文章采用ARIMA模型来实现对天气的有效预测。通过利用ACF和PACF图粗略确定ARIMA模型的参数,最终确定最优模型:ARIMA(1,1,1)为日最低气温模型,其残差序列自相关函数与偏自... 详细信息

由于天气对农业生产、水资源管理和自然灾害预防等具有重要影响,文章采用ARIMA模型来实现对天气的有效预测。通过利用ACF和PACF图粗略确定ARIMA模型的参数,最终确定最优模型:ARIMA(1,1,1)为日最低气温模型,其残差序列自相关函数与偏自相关函数基本落在95%置信区间内;同时Ljung-Box Q统计结果表明残差不存在相关关系(P>0.05),即残差为白噪声,满足随机性假设;最终计算误差(日最低气温)RMSE、MAPE、MAE分别为2.63、1.22%、2.06,预测结果良好,为定西天气的预测提供了可行的方案。

关键词：天气预测时间序列插值法 ARIMA模型

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甘肃省特色农产品展示平台设计与实现

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现代信息科技 2024年第12期8卷 71-75页

作者：李春潇秦立静赵子鹏王虎魁殷正魁甘肃农业大学甘肃兰州730070

目前,我国农业正处于传统农业向现代化农业转型的关键阶段,但却存在对现代技术研发和投入力度不足的问题。为此设计一个小程序,通过简单的点击操作实时展现农田作物生长情况,帮助管理者进行研判并为确保作物正常生长而适时地调整灌溉、... 详细信息

目前,我国农业正处于传统农业向现代化农业转型的关键阶段,但却存在对现代技术研发和投入力度不足的问题。为此设计一个小程序,通过简单的点击操作实时展现农田作物生长情况,帮助管理者进行研判并为确保作物正常生长而适时地调整灌溉、日照等指标。此外,该小程序还可提供产品生产全过程的可视化展示,增加消费者对食品安全的信心。微信小程序具有用户量庞大、开发成本低、绿色环保等优势,运营效益远大于投入成本。

关键词：微信小程序农业农产品平台

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