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Recent advances and applications of single atom catalysts based electrochemical sensors

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Nano Research 2024年第4期17卷 2994-3013页

作者： Mingyue Wang Mingfu Ye Jieyue Wang Yong Xu Zhendong Wang Xinyue Tong Xinya Han Kui Zhang Wenhai Wang Konglin Wu xianwen wei Institute of Clean Energy and Advanced Nanocatalysis(iClean) School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China School of Materials Science and Engineering Anhui University of TechnologyMaanshan 243002China Anhui International Research Center of Energy materials green manufacturing and biotechnology School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China Carbon Cycle and Emission Control Research Center Low-Carbon Research InstituteAnhui University of TechnologyMaanshan 243002China

Single atom catalysts(SACs)have attracted considerable attention due to their unique structures and excellent catalytic performance,especially in the area of catalysis science and energy conversion and storage.In recent years,SACs have emerged as a new type of sensing material for constructing electrochemical sensors(ECSs),presenting excellent sensitivity,selectivity,and stability.Herein,we review the recent advances of SACs in electrochemical sensing and discuss the status quo of current SAC-based ECSs.Specifically,the fundamentals of SAC-based ECSs are outlined,including the involved central metal atoms and various supports of SACs in this field,the detection mechanisms,and improving strategies of SAC-based ECSs.Moreover,the important applications of SAC-based ECSs are listed and classified,covering the detection of reactive oxygen and nitrogen species,environmental pollutants,disease biomarkers,and pharmaceuticals.Last,based on abundant reported cases,the current conundrums of SAC-based ECSs are summarized,and the prediction of their future developing trends is also put forward.

关键词： single atom catalysts(SACs) electrochemical sensors(ECSs) reactive oxygen and nitrogen species environmental pollutants disease biomarkers pharmaceuticals

Cu_(1)-B dual-active sites catalysts for the efficient dehydrogenative coupling and CO_(2)electroreduction

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Nano Research 2023年第4期16卷 4582-4588页

作者： Konglin Wu Zhaobin Fang Cheng Peng Yining Zhang Binbin Jiang Yanshang Kang Zhiming Chen Mingfu Ye Yuxi Wu xianwen wei Shoujie Liu Sha Li Jian Zhang Key Laboratory of Metallurgical Emission Reduction&Resources Recycling of Ministry of Education Anhui University of TechnologyMaanshan 243002China Anhui Laboratory of Clean Catalytic Engineering School of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000China Institute of Clean Energy and Advanced Nanocatalysis(iClean) School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China Chemistry and Chemical Engineering Guangdong Laboratory Shantou 515063China Institute of Molecular Plus Tianjin UniversityTianjin 300072China School of Chemistry and Chemical Engineering Anqing Normal UniversityAnqing 246001China Jiangxi Province Engineering Research Center of Ecological Chemical Industry Jiujiang UniversityJiujiang 332005China College of Chemistry and Materials Engineering Wenzhou UniversityWenzhou 325035China

Dual-active sites(DASs)catalysts have positive potential applications in broad fields because of their specific active sites and synergistic catalytic effects.Therefore,the controllable synthesis and finely regulating the activity of such catalysts has become a hot research area for now.In this work,we developed a pyrolysis-etching-hydrogen activation strategy to prepare the DASs catalysts involving single-atom Cu and B on N-doped porous carbon material(Cu_(1)-B/NPC).Numerous systematic characterization and density functional theoretical(DFT)calculation results showed that the Cu and B existed as Cu-N4 porphyrinlike unit and B-N_(3)unit in the obtained catalyst.DFT calculations further revealed that single-atom Cu and B sites were linked by bridging N atoms to form the Cu_(1)-B-N6 dual-sites.The Cu_(1)-B/NPC catalyst was more effective than the single-active site catalysts with B-N_(3)sites in NPC(B/NPC)and Cu-N4 porphyrin-like sites in NPC(Cu_(1)/NPC),respectively,for the dehydrogenative coupling of dimethylphenylsilane(DiMPSH)with various alcohols,performing the great activity(>99%)and selectivity(>99%).The catalytic performances of the Cu_(1)-B/NPC catalyst remained nearly unchanged after five cycles,also indicating its outstanding recyclability.DFT calculations showed that the Cu_(1)-B-N6 dual-sites exhibited the lowest energy profile on the potential energy surface than that of sole B-N_(3)and Cu-N4 porphyrin-like sites.Furthermore,the rate-limiting step of dehydrogenation of DiMPSH on Cu_(1)-B-N6 dual-sites also showed a much lower activation energy than the other two single sites.Benefitting from the superiority of the Cu_(1)-B-N6 dual-sites,the Cu_(1)-B/NPC catalyst can also be used for CO_(2)electroreduction to produce syngas.Thus,DASs catalysts are promising to achieve multifunctional catalytic properties and have aroused positive attention in the field of catalysis.

关键词： dual-active sites single-atom catalysis porous carbon dehydrogenative coupling

Biomass-assisted approach for large-scale construction ofmulti-functional isolated single-atom site catalysts

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Nano Research 2022年第5期15卷 3980-3990页

作者： Tao Wu Sha Li Shoujie Liu Weng-Chon Cheong Cheng Peng Kai Yao Yingping Li Jieyue Wang Binbin Jiang Zheng Chen Zhiming Chen xianwen wei Konglin Wu Key Laboratory of Metallurgical Emission Reduction&Resources Recycling Ministry of EducationInstitute of Clean Energy and Advanced Nanocatalysis(iClean)School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China Anhui Laboratory of Clean Catalytic Engineering School of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000China Center of Single-Atom Clustersand Nanomaterials(CAN)College of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China Chemistry and Chemical Engineering of Guangdong Laboratory Shantou 515063China Department of Physics and Chemistry Faculty of Science and TechnologyUniversity of MacaoMacaoChina School of Chemistry and Chemical Engineering Anhui Key Laboratory of Photoelectric-Magnetic Functional MaterialsAnqing Normal UniversityAnqing 246011China

In recent years,the isolated single-atom site(ISAS)catalysts have attracted much attention as they are cost-effective,can achieve 100%atom-utilization efficiency,and often display superior catalytic performance.Here,we developed a biomass-assisted pyrolysis-etching-activation(PEA)strategy to construct ISAS metal decorated on N and B co-doped porous carbon(ISAS M/NBPC,M=Co,Fe,or Ni)catalysts.This PEA strategy can be applied in the universal and large-scale preparation of ISAS catalysts.Interestingly,the ISAS M/NBPC(M=Co,Fe,or Ni)catalysts show multi-functional features and excellent catalytic activities.They can be used to conduct different types of catalytic reactions,such as O-silylation(OSI),oxidative dehydrogenation(ODH),and transfer hydrogenation(THG).In addition,we used the transfer hydrogenation of nitrobenzene as a typical reaction and revealed the difference between ISAS Co/NBPC and ISAS Co/NPC(N-doped porous carbon)catalysts by density functional theory(DFT)calculations,and which showed that the decreased barrier of the ratedetermining step and the low-lying potential energy diagram indicate that the catalytic activity is higher when ISAS Co/NBPC is used than that when ISAS Co/NPC is used.These results demonstrate that the catalytic performance can be effectively improved by adjusting the coordination environment around the ISAS.

关键词： single-atom site multifunctional catalyst heteroatomic coordination oxydehydrogenation hydrogenation

Rationally engineered Co and N co-doped WS_(2) as bifunctional catalysts for pH-universal hydrogen evolution and oxidative dehydrogenation reactions

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Nano Research 2022年第3期15卷 1993-2002页

作者： Min Ling Na Li Binbin Jiang Renyong Tu Tao Wu Pingli Guan Yin Ye Weng-Chon(Max)Cheong Kaian Sun Shoujie Liu Konglin Wu Aijian Huang xianwen wei College of Chemistry and Materials Science Key Laboratory of Electrochemical Clean Energy of Anhui Higher Education InstitutesKey Laboratory of Functional Molecular Solidsthe Ministry of EducationAnhui Normal UniversityWuhu 241002China School of Chemistry and Chemical Engineering Institute of Clean Energy and Advanced Nanocatalysis(iClean)Anhui Province Key Laboratory of Coal Clean Conversion and High Valued UtilizationAnhui University of TechnologyMaanshan 243002China School of Chemistry and Chemical Engineering Anhui Key Laboratory of Photoelectric-Magnetic Functional MaterialsAnqing Normal UniversityAnqing 246011China Department of Chemistry Tsinghua UniversityBeijing 100084China Department of Physics and Chemistry Faculty of Science and TechnologyUniversity of MacaoMacaoChina Chemistry and Chemical Engineering of Guangdong Laboratory Shantou 515063China School of Electronics Science and Engineering University of Electronic Science and Technology of ChinaChengdu 610054China

In the field of electrolysis of water,the design and synthesis of catalysts over a wide pH range have attracted extensive attentions.In this paper,Co and N are co-introduced into the structural unit of tungsten disulfide(WS_(2)),and the hydrogen evolution reaction(HER)performances of different WS_(2)-based catalysts are theoretically predicted and systematically studied by density functional theory(DFT)calculations.With the guidance of DFT calculations,an evaporation-pyrolysis strategy is applied to prepare Co and N co-doped WS_(2)(Co,N-WS_(2))flower-like nanosheets,which exhibits excellent HER performance over a wide pH range.In addition,the DFT calculations show that the active sites in Co,N-WS_(2) have a good ability of hydrogen adsorption after the introduction of Co and N,suggesting that such a co-doping system will be an ideal catalyst for oxidative dehydrogenation(ODH).The following experiment results indeed evidence that the Co,N-WS_(2) catalyst displays a high activity in the ODH of 1,2,3,4-tetrahydroquinoline(4H-quinoline)and its derivatives.Therefore,this work provides a good example for the rational design and accurate preparation of functional catalysts,which enables it possible to develop other efficient catalysts with multiple functions.

关键词： WS2 heteroatomic doping bifunctional catalyst density functional theory(DFT)calculation electrolysis of water

Copper single-atom catalysts with photothermal performance and enhanced nanozyme activity for bacteria-infected wound therapy

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Bioactive Materials 2021年第12期6卷 4389-4401页

作者： xianwen Wang Qianqian Shi Zhengbao Zha Dongdong Zhu Lirong Zheng Luoxiang Shi xianwen wei Lian Lian Konglin Wu Liang Cheng Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-based Functional Materials and DevicesSoochow UniversitySuzhou215123PR China School of Food and Biological Engineering Hefei University of TechnologyHefei230009PR China Institute of Clean Energy and Advanced Nanocatalysis School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan243002PR China Beijing Synchrotron Radiation Facility(NSRF) Institute of High Energy PhysicsChinese Academy of ScienceBeijing100049China Department of Oncology Suzhou Xiangcheng People’s HospitalSuzhou215131China

Nanozymes have become a new generation of antibiotics with exciting broad-spectrum antibacterial properties and negligible biological toxicity.However,their inherent low catalytic activity limits their antibacterial properties.Herein,Cu single-atom sites/N doped porous carbon(Cu SASs/NPC)is successfully constructed for photothermal-catalytic antibacterial treatment by a pyrolysis-etching-adsorption-pyrolysis(PEAP)strategy.Cu SASs/NPC have stronger peroxidase-like catalytic activity,glutathione(GSH)-depleting function,and photothermal property compared with non-Cu-doped NPC,indicating that Cu doping significantly improves the catalytic performance of nanozymes.Cu SASs/NPC can effectively induce peroxidase-like activity in the presence of H2O2,thereby generating a large amount of hydroxyl radicals(•OH),which have a certain killing effect on bacteria and make bacteria more susceptible to temperature.The introduction of near-infrared(NIR)light can generate hyperthermia to fight bacteria,and enhance the peroxidase-like catalytic activity,thereby generating additional•OH to destroy bacteria.Interestingly,Cu SASs/NPC can act as GSH peroxidase(GSH-Px)-like nanozymes,which can deplete GSH in bacteria,thereby significantly improving the sterilization effect.PTT-catalytic synergistic antibacterial strategy produces almost 100%antibacterial efficiency against Escherichia coli(E.coli)and methicillin-resistant Staphylococcus aureus(MRSA).In vivo experiments show a better PTT-catalytic synergistic therapeutic performance on MRSA-infected mouse wounds.Overall,our work highlights the wide antibacterial and anti-infective bio-applications of Cu single-atom-containing catalysts.

关键词： Copper single-atom catalysts Nanozymes Photothermal therapy Antibacterial Catalytic therapy

一种喹啉类分子对硝基芳香化合物和阴离子的荧光传感研究

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化学通报 2024年第6期87卷 726-731,719页

作者：张莉艳徐志超魏先文安徽工业大学化学与化工学院马鞍山243032

以2-(1H-苯并[d]咪唑基)-8-羟基喹啉和2-氯甲基吡啶盐酸盐为原料合成了一种喹啉类功能分子(BIPQ),相比其他有机溶剂,化合物BIPQ的N,N-二甲基乙酰胺溶液在452nm显示出最强荧光发射。硝基芳香化合物2,4,6-三硝基苯酚(TNP)和阴离子Cr_(2)O_... 详细信息

以2-(1H-苯并[d]咪唑基)-8-羟基喹啉和2-氯甲基吡啶盐酸盐为原料合成了一种喹啉类功能分子(BIPQ),相比其他有机溶剂,化合物BIPQ的N,N-二甲基乙酰胺溶液在452nm显示出最强荧光发射。硝基芳香化合物2,4,6-三硝基苯酚(TNP)和阴离子Cr_(2)O_(7)^(2-)对BIPQ的荧光表现出明显的猝灭效应,猝灭常数KSV分别为5.9×10^(3)L/mol和3.8×10^(3)L/mol。BIPQ在荧光检测TNP和Cr_(2)O_(7)^(2-)过程中对其他硝基芳香化合物和阴离子表现出很好的抗干扰能力。此外,本文还研究了化合物BIPQ有效荧光检测TNP和Cr_(2)O_(7)^(2)-的溶液pH范围,并将BIPQ用于实际水样中TNP和Cr_(2)O_(7)^(2)-的荧光检测。

关键词：喹啉类分子三硝基苯酚 Cr2O72-离子荧光传感

C_(60)-MoP-C纳米花范德瓦耳斯异质结及其电催化析氢性能

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无机化学学报 2024年第4期40卷 771-781页

作者：李文江关平丽余锐程源晟魏先文安徽师范大学化学与材料科学学院功能分子固体教育部重点实验室芜湖241000 安徽工业大学化学与化工学院材料科学与工程研究院煤清洁转化与高值化利用安徽省重点实验室马鞍山243002

采用气固法制备了磷化钼-碳纳米花(MoP-CFs),通过简单的超声自组装将C_(60)修饰在MoP-CFs表面,形成范德瓦耳斯异质结。研究其电催化析氢性能发现,C_(60)的修饰能够有效降低电催化析氢过电位。其中,10%C_(60)-MoP-CFs样品(10%为C_(60)的... 详细信息

采用气固法制备了磷化钼-碳纳米花(MoP-CFs),通过简单的超声自组装将C_(60)修饰在MoP-CFs表面,形成范德瓦耳斯异质结。研究其电催化析氢性能发现,C_(60)的修饰能够有效降低电催化析氢过电位。其中,10%C_(60)-MoP-CFs样品(10%为C_(60)的质量分数)表现出最佳催化活性,在酸性和碱性条件下达到10 mA·cm^(-2)的电流密度时,所需要的过电位分别为158和157 mV,并且具有至少20 h的电催化稳定性。C_(60)与MoP-CFs之间强电子耦合作用促进电子由C_(60)迁移到MoP-CFs表面,有助于减小电荷传输阻力,加快电催化析氢界面反应动力学过程。

关键词：富勒烯能量转换多相催化电化学制氢绿色化学

基于区间分块Q学习的智能车辆安全舒适刹车算法

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计算机应用研究 2024年第1期41卷 183-187页

作者：余欣磊周贤文张依恋顾伟上海海事大学航运技术与控制工程交通行业重点实验室上海201306

针对当前智能汽车刹车场景下的安全与舒适性问题,提出一种基于区间分块的Q学习算法。首先在Q表中将前车加速度以一定间隔划分入等长区间,用区间中值做间隔来划分后车加速度。其次通过在安全条件下与加速度呈负相关的奖励设置,使智能体... 详细信息

针对当前智能汽车刹车场景下的安全与舒适性问题,提出一种基于区间分块的Q学习算法。首先在Q表中将前车加速度以一定间隔划分入等长区间,用区间中值做间隔来划分后车加速度。其次通过在安全条件下与加速度呈负相关的奖励设置,使智能体在保证安全的前提下尽量降低刹车加速度。最后在智能体训练的过程中遵循ε-贪心策略以减少随机性,在训练完毕后遵循贪心策略以最大程度利用智能体。将提出的算法与传统Q学习算法在三种常见道路场景上进行仿真测试。实验结果显示使用提出算法的智能车辆在刹车场景中安全率100%、平均刹车加速度小于2 m/s~2且能处理连续刹车加速度,表明提出的算法能够在确保智能汽车安全刹车的同时实现较低的刹车加速度。同时在连续刹车加速度与离线环境等复杂情况下,算法均能正常使用。

关键词：智能汽车智能刹车 Q学习区间分块

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基于HS-GC-MS的降香真伪鉴别

中国实验方剂学杂志 2024年第2期30卷 156-163页

作者：赵莉孟晓伟李家荣朱清危先文刘荣华陈兰英江西中医药大学药学院南昌330004 江西中医药大学中药固体制剂制造技术国家工程研究中心南昌330006

目的:通过对降香及伪品中挥发性成分分析,筛选其挥发性差异成分,为降香真伪鉴别提供依据。方法:采用顶空气相色谱-质谱法(HS-GC-MS)检测降香及伪品中挥发性成分,GC条件采用程序升温(柱箱初始温度50℃,保留时间1 min,以10℃·min^(-1)升... 详细信息

目的:通过对降香及伪品中挥发性成分分析,筛选其挥发性差异成分,为降香真伪鉴别提供依据。方法:采用顶空气相色谱-质谱法(HS-GC-MS)检测降香及伪品中挥发性成分,GC条件采用程序升温(柱箱初始温度50℃,保留时间1 min,以10℃·min^(-1)升温至300℃保持10 min),流速1.0 mL·min^(-1),分流比10∶1,进样量1 mL,采用电子轰击离子源(EI),扫描范围m/z 35~550。通过数据库匹配鉴定化合物种类,利用峰面积归一法计算各成分相对质量分数,并运用SIMCA 14.1软件对检测结果进行主成分分析(PCA)、正交偏最小二乘法-判别分析(OPLS-DA)与聚类分析,根据变量重要性投影(VIP)值>2及P<0.05筛选出降香及伪品的挥发性差异成分。结果:分别从降香、巴里黄檀、阔叶黄檀、两粤黄檀、斜叶黄檀、交趾黄檀中鉴定出26、17、8、22、24、7个挥发性成分,其中降香的特有成分11种,巴里黄檀特有挥发性成分6种、阔叶黄檀特有挥发性成分3种、两粤黄檀特有挥发性成分6种、斜叶黄檀特有挥发性成分8种、交趾黄檀特有挥发性成分4种。PCA结果显示,除阔叶黄檀与交趾黄檀不能明显区分外,降香与其他伪品均能各自分布在一定的区域内;OPLS-DA结果显示,降香及5种伪品各自聚为一类,表明降香与伪品挥发性成分具有明显差异性,最终共筛选出31个降香与其伪品的挥发性成分差异标志物。结论:HS-GC-MS结合SIMCA 14.1软件可以系统阐释降香与其伪品中挥发性差异成分,适用于降香及伪品的快速鉴别研究。

关键词：降香真伪鉴别顶空气相色谱-质谱法(HS-GC-MS) 挥发性成分主成分分析(PCA) 正交偏最小二乘法判别分析(OPLS-DA)