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Recent advances and applications of single atom catalysts based electrochemical sensors

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

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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

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Cobalt-free Composite Ba_(0.5)Sr_(0.5)Fe_(0.9)Ni_(0.1)O_(3-δ)-Ce_(0.8)Sm_(0.2)O_(2-δ) as Cathode for Intermediate-Temperature Solid Oxide Fuel Cell

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Journal of Materials Science & Technology 2012年第9期28卷 828-832页

作者： Xiangfeng Chu Feng Liu Weichang Zhu Yongping Dong mingfu ye Wenqi Sun School of Chemistry and Chemical Engineering Anhui University of TechnologyMaanshan 243002China School of Materials Science and Engineering Anhui University of TechnologyMaanshan 243002China

New cobalt-free composites consisting of Ba0.5Sr0.5Fe0.9Ni0.1O3-δ （BSFN） and Ce0.8Sm0.2O2-δ （SDC） were investigated as possible cathode materials for intermediate-temperature solid oxide fuel cell （IT-SOFC）. BSFN, which was synthesized by auto ignition process, was chemically compatible with SDC up to 1100 ℃ as indicated by X-ray diffraction analysis. The electrical conductivity of BSFN reached the maximum value of 57 S.cm-1 at 450 ℃. The thermal expansion coefficient （TEC） value of BSFN was 30.9×10-6 K-1, much higher than that of typical electrolytes. The electrochemical behavior of the composites was analyzed via electrochemical impedance spectroscopy with symmetrical cells BSFN-SDC/SDC/BSFN-SDC. The area specific interracial polarization resistance （ASR） decreased with increasing SDC content of the composite. The area specific interracial polarization resistance （ASR） at 700 ℃ is only 0.49, 0.34 and 0.31 Ω.cm2 when 30, 40, and 50 wt% SDC was cooperated to BSFN, respectively. These results suggest that BSFN-SDC is a possible candidate for IT-SOFC cathode.

关键词： Ba0.5Sr0.5Fe0.9Ni0.1O3- δ Cathode Intermediate-temperature solid oxide fuel cell （IT-SOFC） Solid oxide fuel cell

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Photovoltaic molecules based on vinylene-bridged oligothiophene applied for bulk-heterojunction organic solar cells

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Journal of Energy Chemistry 2018年第2期27卷 426-431页

作者： Jing Zhang Pan Yin Linjun Xu Ping Shen mingfu ye Ningyi Yuan Jianning Ding School of Material Science & Engineering Jiangsu Collaborative Innovation Center of Photovoltaic Science & Engineering Changzhou University Changzhou 213164 Jiangsu China College of Chemistry and Key Laboratory of Environmentally Friendly Chemistry and Applications of Ministry of Education Xiongtan University Xiangtan 411105 Hunan China School of Chemistry and Chemical Engineering Anhui University of Technology Maanshan 243002 Anhui China

We have synthesized two photovoltaic molecules（HEX-3TVT-ID and EH-3TVT-ID） based on vinylenebridged oligothiophene applied as donor for the solution-processable bulk-heterojunction organic solar cells（OSCs）. Vinylene unit was introduced as π-bridge in the oligothiophenes with 1,3-indenedione as end group and 4,4’-dihexyl-2,2’：5’,2’-terthiophene or 3’,4’-di（octan-3-yl）-2,2’：5’,2’-terthiophene as core,respectively. Due to the different substituent positions of the alkyl group relative to the vinylene unit in the terthiophene, HEX-3TVT-ID and EH-3TVT-ID show different optical and electrochemical properties, corresponding to the photovoltaic performance of the OSCs devices. The power conversion efficiency（PCE） of the OSCs based on a blend of HEX-3TVT-ID and PC71BM（1：0.8, weight ratio, 0.5% CN） reached 2.3%. In comparison, the OSCs based on the blend of EH-3TVT-ID and PC71BM in the weight ratio of 1：1 without the additive show a higher PCE of 2.7%, with a typically high VOC of 0.93 V, under the illumination of AM 1.5, 100 mW cm-2.

关键词： Organic solar cells Photovoltaic organic molecules Vinylene-bridged oligothiophene

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NiPd/TiO_(2)催化剂的制备及催化甲酸分解制氢

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精细化工 2024年第6期41卷 1302-1309页

作者：吴慧郑君宁左佑华许立信叶明富万超安徽工业大学化学与化工学院安徽马鞍山243000 南开大学先进能源材料化学教育部重点实验室天津300071 宁德师范学院绿色能源与环境催化福建高校重点实验室福建宁德352100 常州大学江苏省绿色催化材料与技术重点实验室江苏常州213164 浙江大学化学工程与生物工程学院浙江杭州310058

高效、清洁且无毒无害的催化剂是实现以甲酸(HCOOH)为化学储氢材料分解制氢的重点。首先,通过水热法453 K下制备了TiO_(2)载体;然后,通过浸渍法将活性组分Ni、Pd负载到TiO_(2)载体上合成了NiPd/TiO_(2)催化剂。采用SEM、TEM、N2吸附-脱... 详细信息

高效、清洁且无毒无害的催化剂是实现以甲酸(HCOOH)为化学储氢材料分解制氢的重点。首先,通过水热法453 K下制备了TiO_(2)载体;然后,通过浸渍法将活性组分Ni、Pd负载到TiO_(2)载体上合成了NiPd/TiO_(2)催化剂。采用SEM、TEM、N2吸附-脱附、XRD、XPS、UV-Vis DRS对催化剂样品进行了表征。探究了由不同n(Ni)∶n(Pd)制备的催化剂对催化甲酸分解制氢性能的影响。结果表明,NiPd金属粒子对TiO_(2)的改性不仅扩大了TiO_(2)的光吸收范围,还有助于电荷分离,加速光催化反应的进行。在光照下,当NiPd/TiO_(2)催化剂中n(Ni)∶n(Pd)=2∶8时,催化剂的反应转化频率(TOF)最大,为3528 h^(–1)(323 K下),甲酸分解的活化能(E_(a))为53.9 kJ/mol。

关键词： NiPd催化剂甲酸分解制氢 TiO_(2) 光照

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层状多孔炭片负载钌催化剂的制备及其催化氨硼烷水解制氢性能研究

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燃料化学学报（中英文） 2024年第3期52卷 429-437页

作者：左佑华吴慧花俊峰郑君宁许立信叶明富万超安徽工业大学化学与化工学院安徽马鞍山243000 浙江省环境科技有限公司浙江杭州310027 南开大学先进能源材料化学教育部重点实验室天津300071 宁德师范学院绿色能源与环境催化福建高校重点实验室福建宁德352100 常州大学江苏省绿色催化材料与技术重点实验室江苏常州213164 浙江大学化学工程与生物工程学院浙江杭州310058

本研究以煤沥青为炭材料,氯化钠为模板剂,碳酸钾为活化剂,在氩气气氛下高温煅烧得到载体层状多孔炭片(LPCS),通过浸渍法向其中加入RuCl3金属溶液,将活性组分Ru负载到LPCS载体上合成Ru/LPCS催化剂,并对其催化氨硼烷水解制氢的性能进行了... 详细信息

本研究以煤沥青为炭材料,氯化钠为模板剂,碳酸钾为活化剂,在氩气气氛下高温煅烧得到载体层状多孔炭片(LPCS),通过浸渍法向其中加入RuCl3金属溶液,将活性组分Ru负载到LPCS载体上合成Ru/LPCS催化剂,并对其催化氨硼烷水解制氢的性能进行了研究。结果表明,Ru/LPCS催化剂中,当煅烧温度为1123 K时,Ru的负载量为2%时,催化剂的反应转化频率(TOF)值最大,此时有光下催化剂的TOF为334.8 min^(-1),是无光照时TOF的1.38倍。在光照下,催化剂的活化能(Ea)从90.60 kJ/mol下降到70.33 kJ/mol。氨硼烷水解制氢速率相对于其浓度的级数为0.75,而相对于催化剂的用量满足于一级动力学关系。

关键词：钌基催化剂氨硼烷水解制氢层状多孔炭片

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N-羟基琥珀酰亚胺作为(pq)_(2)Ir(acac)共反应剂电致化学发光法检测Hg^(2+)

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分析试验室 2024年第5期43卷 642-648页

作者：付云峰任美娟吴芳辉叶明富殷国霞王晨安徽工业大学化学与化工学院马鞍山243000 生物膜法水质净化及利用技术教育部工程研究中心安徽工业大学建筑工程学院马鞍山243000 信息材料及器件化应用四川省高校重点实验室成都信息工程大学成都610225

制备了(pq)_(2)Ir(acac)(pq=2-苯基喹啉,acac=乙酰丙酮)并对其进行表征。采用N-羟基琥珀酰亚胺(NHS)作为中性混合溶剂中(pq)_(2)Ir(acac)的共反应剂,获得强的电致化学发光(ECL)信号。向该体系中加入Hg^(2+)后,因NHS与Hg^(2+)的特异性螯... 详细信息

制备了(pq)_(2)Ir(acac)(pq=2-苯基喹啉,acac=乙酰丙酮)并对其进行表征。采用N-羟基琥珀酰亚胺(NHS)作为中性混合溶剂中(pq)_(2)Ir(acac)的共反应剂,获得强的电致化学发光(ECL)信号。向该体系中加入Hg^(2+)后,因NHS与Hg^(2+)的特异性螯合作用,阻断了NHS与(pq)_(2)Ir(acac)之间的共反应,使得其ECL响应显著降低,据此构建了灵敏检测Hg^(2+)的方法。优化条件下,(pq)_(2)Ir(acac)/NHS体系ECL强度变化的对数值与Hg^(2+)浓度的自然对数值在0.1~90μmol/L范围内呈良好的线性关系,检出限达33 nmol/L。(pq)_(2)Ir(acac)/NHS体系对Hg^(2+)具有良好的选择性和稳定性。该方法可用于测定实际水样中Hg^(2+)浓度。

关键词：环金属铱配合物 N-羟基琥珀酰亚胺电致化学发光汞离子检测

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双模板剂合成CO_(2)P纳米片及其催化氨硼烷水解性能的研究

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石油炼制与化工 2024年第2期55卷 186-192页

作者：孙佳丽郑君宁花俊峰邱小魁许立信叶明富万超安徽硅宝有机硅新材料有限公司安徽马鞍山243000 安徽工业大学化学与化工学院浙江省环境科技有限公司南开大学先进能源材料化学教育部重点实验室宁德师范学院绿色能源与环境催化福建高校重点实验室浙江大学化学工程与生物工程学院常州大学江苏省绿色催化材料与技术重点实验室

开发一种在温和条件下具有高活性、高选择性的催化剂是实现氨硼烷水解制氢应用的关键。以构建具有P掺杂材料为出发点,以两种不同比例的金属盐作为模板剂,以过渡非贵金属Co为中心金属,合成出制作方法简便、性能优异的催化剂。通过乙酸钴... 详细信息

开发一种在温和条件下具有高活性、高选择性的催化剂是实现氨硼烷水解制氢应用的关键。以构建具有P掺杂材料为出发点,以两种不同比例的金属盐作为模板剂,以过渡非贵金属Co为中心金属,合成出制作方法简便、性能优异的催化剂。通过乙酸钴和氨水制备出Co_(3)O_(4)前躯体,将Co_(3)O_(4)前躯体与NaH_(2)PO_(2),NaCl,LiCl混合,在N_(2)气氛下焙烧,然后进行水洗将两种盐模板剂去除,得到纳米片催化剂CO_(2)P-NaLi。试验结果表明,当n(NaCl)∶n(LiCl)=1∶0.15时制备的催化剂CO_(2)P-NaLi_(0.15)催化活性最高,其在298 K、光照条件下催化氨硼烷水解反应的初始转化率(TOF)为31.2 min^(-1),且该催化剂上氨硼烷分解的活化能(E_(a))为60.8 kJ/mol。循环5次后,催化剂依然保持良好活性,表明其拥有良好的稳定性。

关键词：磷化钴氨硼烷储氢材料盐模板剂法

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Experimental study of core MHD behavior and a novel algorithm for rational surface detection based on profile reflectometry in EAST

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Plasma Science and Technology 2024年第3期26卷 66-75页

作者：叶凯萱周振张涛马九阳王嵎民李恭顺耿康宁吴茗甫文斐黄佳张洋邵林明杨书琪钟富彬高善露喻琳周子强向皓明韩翔张寿彪李国强高翔 the EAST Team Institute of Plasma Physics Hefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031People's Republic of China University of Science and Technology of China Hefei 230026People's Republic of China Hebei Key Laboratory of Compact Fusion Langfang 065001Peoples Republic of China ENN Science and Technology Development Co. Ltd.Langfang 065001Peoples Republic of China Advanced Energy Research Center Shenzhen UniversityShenzhen 518060People's Republic of China

Microwave reflectometry is a powerful diagnostic that can measure the density profile and localized turbulence with high spatial and temporal resolution and will be used in ITER,so understanding the influence of plasma perturbations on the reflect signal is important.The characteristics of the reflect signal from profile reflectometry,the time-of-flight(TOF)signal associated with the MHD instabilities,are investigated in EAST.Using a 1D full-wave simulation code by the Finite-DifferenceTime-Domain(FDTD)method,it is well validated that the local density flattening could induce the discontinuity of the simulated TOF signal and an obvious change of reflect amplitude.Experimental TOF signals under different types of MHD instabilities(sawtooth,sawtooth precursors and tearing mode)are studied in detail and show agreement with the simulation.Two new improved algorithms for detecting and localizing the radial positions of the low-order rational surface,the cross-correlation and gradient threshold(CGT)method and the 2D convolutional neural network approach(CNN)are presented for the first time.It is concluded that TOF signal analysis from profile reflectometry can provide a straightforward and localized measurement of the plasma perturbation from the edge to the core simultaneously and may be a complement or correction to the q-profile control,which will be beneficial for the advanced tokamak operation.

关键词： MHD instabilities profile reflectometry rational surface detection convolutional neural network(CNN) EAST tokamak

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Bonding Efficacy of a Self-adhesive Resin Cement to Enamel and Dentin

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Journal of Wuhan University of Technology(Materials Science) 2014年第6期29卷 1307-1312页

作者：王林虎 XU Haixing LI Songyang 施斌 LI Rong ye mingfu YANG Jing Department of Implantology Hospital of Stomatology Wuhan University Department of Pharmaceutical Engineering School of Chemistry Chemical Engineering and Life Sciences Wuhan University of Technology Department of Biology Hongkong Baptist University

With the objective to evaluate the bonding efficacy of a new self-adhesive resin cement（RelyX Unicem, 3M ESPE） to enamel and dentin using a shear bonding strengths test with or without acid etching pretreatment, flat buccal dentin surface and mesial/distal enamel surface were made using a high-speed diamond bur. Copper rings were luted using Rely X Unicem（RU; 3M ESPE）, Panavia F（PF; Kuraray） or Vitique（VI; DMG）. For RU, the shear bonding strengths using GL（Gluma Etch, Heraeus） acid etching pretreatment were also tested. The teeth were placed into copper rings（inner diameter： 16 mm, height： 4mm） and embedded in methylmethacrylate resin. The specimens were stored for 24 h in distilled water at 37 ℃ prior to shear bonding strengths testing. In addition, bond failures were examined by optical microscope and categorized as 4 models such as different adhesive, cohesive, or mixed. Shear bonding strengths were calculated by dividing the maximum debonding force over the cross sectional area of each specimen. The Kruskal-Wallis test was used to determine pairwise statistical differences（P 〈 0.05） in SBS between the experimental groups. For dentin bonding strength, statistical analysis showed that there was no significant difference among RU（12.84 MPa）, PF（14.93 MPa） and VI（11.03 MP）; and the bonding strengths of them were higher than RU with acid etching pretreatment（9.12 MP）. When bonded to enamel, PF（17.99 MP） and VI（17.58 MP） scored significantly higher than RU efficacy.The use of self-adhesive cement Rely X Unicem can obtain the bonding strengths to dentin similar to traditional resin cements. Phosphoric acid etching can improve the bonding strengths of the selfadhesive resin cement to enamel, but was negative for dentin.

关键词： RelyX Unicem dentin enamel shear bond strength

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