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Facet and dimensionality control of Pt nanostructures for efficient oxygen reduction and methanol oxidation electrocatalysts

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Nano Research 2016年第9期9卷 2811-2821页

作者： Lingzheng Bu Yonggang Feng jianlin yao Shaojun Guo Jun Guo Xiaoqing Huang College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Department of Materials Science and Engineering & Department of Energy and Resources Engineering College of EngineeringPeking UniversityBeijing 100871China Testing & Analysis Center Soochow UniversitySuzhou 215123China

The control of the size, composition, and shape of platinum nanocrystals has attracted much attention recently, mostly due to their unique properties and related catalytic functionalities. However, the realization of platinum nanocrystals with controlled exposed facets and dimensionality remains a significant challenge. Herein, we show an efficient synthetic strategy to selectively prepare highly controllable platinum nanocrystals with distinct dimensionalities from onedimensional nanowires to zero-dimensional octahedra. Although the synthesis of platinum nanowires has been reported multiple times, the synthetic approach reported herein is much more novel and robust and ultimately results in high yields of high-quality platinum nanowires. Such dimensionality tuning on {111} facet dominated platinum nanocrystals allows us to firstly investigate the effect of the number of edges/corners on the electrocatalytic properties. Our results show that the synthesized platinum nanocrystals exhibit very interesting dimensionality-dependent electrocatalytic activity towards both the oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR), in which one-dimensional platinum nanowires with minimized edges/corners show enhanced electrocatalytic activities with respect to zero-dimensional platinum octahedra. Our dimensionality tuning also provides Pt nanowires with superior durability for the oxygen reduction reaction with negligible activity decay over the course of 30,000 potential sweeps. The present work highlights that the {111} facet bound platinum nanowires with minimized edges/corners are indeed promising candidates as electrocatalysts with excellent activity and superior durability. [Figure not available: see fulltext.] © 2016, Tsinghua University Press and Springer-Verlag Berlin Heidelberg.

关键词： platinum nanowires octahedra {111} facet oxygen reduction reaction methanol oxidation reaction

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S-,P-stabilized bromoallenes for modular allenylborylation of alkenes

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Science China Chemistry 2024年第1期67卷 360-367页

作者： Jixin Wang Donghao Luo Ying Hu Zhili Duan jianlin yao Konstantin Karaghiosoff Jie Li Key Laboratory of Organic Synthesis of Jiangsu Province Suzhou Key Laboratory of Pathogen Bioscience and Anti-infective MedicineCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Department Chemie Ludwig-Maximilians-Universitat MunchenButenandtstr.5-13Haus F81377 MunichGermany State Key Laboratory and Institute of Elemento-Organic Chemistry Haihe Laboratory of Sustainable Chemical TransformationsCollege of ChemistryNankai UniversityTianjin 300071China

Simultaneously forming a carbon-carbon and a carbon-heteroatom bond in a single step through transition metal-catalyzed alkene difunctionalization strategy has emerged as a powerful tool for synthetic organic *** to the uncontrollable reactivity,direct cross-coupling with bromoallenes as the building blocks for the selective allenation and borylation remains *** herein report a new type of S-and P-stabilized bromoallenes for palladium-catalyzed modular allenation and borylation of alkenes to the divergent synthesis of multiply functionalized allenes in a highly regio-and diastereoselective *** reaction features broad substrate scope and wide functional group compatibility,thus providing a straightforward method to install allenyl and boryl groups across *** experiments highlight the crucial importance of S-,P-stabilization for the oxidative insertion of Pd-species into the allenyl-Br *** facile syntheses of bioactive allenic steroids and exocyclic allenes demonstrate the synthetic utility of this protocol.

关键词： alkene difunctionalization olefins bromoallenes allenylborylation palladium

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Structure of water at ionic liquid/Ag interface probed by surface enhanced Raman spectroscopy

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Science China Chemistry 2011年第1期54卷 200-204页

作者： NIU TianChao YUAN YaXian yao jianlin LU Feng GU RenAo College of Chemistry Chemical Engineering and Material Science Soochow University Suzhou 215123 China

The potential-dependent adsorption behavior of water and ionic liquid was probed by surface-enhanced Raman spectroscopy （SERS） at the Ag electrode surface in the ionic liquids containing water with different concentrations. The configuration of water at the ionic liquid/electrode interface and the relationship between the potential of zero charge （pzc） and the molar frac- tion of water were deduced through the changes in the vibrational frequency of OH stretching mode. A small Stark effect value was determined in the system with lower molar fraction of water. With the increase of the water concentration, the OH stretching vibrational frequency gradually shifted to the high wavenumber region, the pzc was also moved positively, and the Stark effect value of OH stretching vibrational mode increased. It reached about 76 cm-1 V-I in the 1 tool L-1 [BMIM]Br aqueous solution. These differences were mainly contributed by hydrogen bonding and the configuration of water in the ionic liquid solution. In the solution with lower water content, water molecules existed at the interface layer through hydrogen bond- ing with cations, while in the higher content solution, the intermolecular hydrogen bonding between water molecules was strengthened and the possibility of the direct interaction between the water molecule and electrode surface increased.

关键词： water ionic liquid Ag electrode interface surface enhanced Raman spectroscopy

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SERS mechanism of nickel electrode

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Chinese Science Bulletin 2002年第23期47卷 1983-1986页

作者： YANG Zhilin WU Deyin yao jianlin HU Jianqiang REN Bin ZHOU Haiguang TIAN Zhongqun State Key Laboratory for Physical Chemistry of Solid Surfaces Department of ChemistryXiamen UniversityXiamen 361005China Department of Physics Xiamen UniversityXiamen 361005China

Based on the theoretical model for the two-dimensional arrays, the dependence of the surface-enhanced Raman scattering (SERS) effect of nickel electrode, especially the ordered two-dimensional nanowires, on the incident photon energy in the range of 0.6-4.0 eV are analyzed, and most of the works are focused on the effect of the shape of nano-particles. The theoretical analysis shows that nickel can exhibit weak surface-enhanced Raman scattering effect when the surface is roughened properly, and the enhancement factor is about 102-104. Compared to the typical highly SERS-active Ag substrate, the SERS of nickel does not show the character of surface plasma resonance of the metal. The calculated result shows that the lightning-rod effect contributes the most to the SERS of Ni nanowires in the EM mechanism. The theoretical prediction is in good agreement with the experimental result qualitatively and may be instructive to finding a new method to fabricate the SERS-active transition-metal substrate.

关键词： surface-enhanced Raman scattering two-dimensional arrays of spheroids lightning-rod effect transition metals nickel.

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Nickel-catalyzed regiodivergent syn-hydrosilylation of disubstituted alkynes

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Science Bulletin 2024年第21期69卷 3334-3339页

作者： Jixin Wang Jie Lin Zhili Cui jianlin yao Konstantin Karaghiosoff Jie Li Key Laboratory of Organic Synthesis of Jiangsu Province Suzhou Key Laboratory of Pathogen Bioscience and Anti-infective MedicineCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Department Chemie Ludwig-Maximilians-Universität MünchenMunich 81377Germany

Given the importance of alkenylsilanes in organosilicon chemistry and material science, direct transition-metal-catalyzed selective hydrosilylation of alkynes with hydrosilanes has emerged as apowerful platform for accessing such building blocks in a straightforwardand atom-economical fashion [1,2]. Among them,regio- and stereoselective hydrosilylations of terminal alkynesand symmetrical internal alkynes have been thoroughly studied,and a range of 3d transition-metal catalysts exhibited excellentb-(E), b-(Z), and a-selectivity in these transformations [3–9].Despite these major advances, crucial drawbacks exist in thecatalytic hydrosilylation between hydrosilanes and unsymmetricalinternal alkynes, particularly when done in a regiodivergent andstereocontrolled fashion. The representative examples are largelyrestricted to the use of electronically [10] or sterically [11] biasedalkynes (Fig. 1a).

关键词： catalyzed alkynes substituted

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表面增强拉曼光谱在非水体系中的研究进展

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光谱学与光谱分析 1999年第4期19卷 531-534页

作者：顾仁敖曹佩根姚建林苏州大学化学系厦门大学固体表面物理化学国家重点实验室

本文论述了表面增强拉曼光谱（ＳＥＲＳ）在非水体系中的研究历史、现状及应用前景，系统阐述了非水体系固／液界面结构、无机离子和有机分子的吸附以及非水电极过程方面ＳＥＲＳ技术的研究进展。

关键词：表面增强非水体系 SERS 拉曼普

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基于表面增强拉曼光谱快速检测纺织品禁用染料

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高等学校化学学报 2021年第12期42卷 3716-3721页

作者：潘菁徐敏敏袁亚仙姚建林苏州大学材料与化学化工学部苏州215123

基于表面增强拉曼光谱(SERS)技术,发展了一种纺织品中染料定性检测的快速方法.以国家明确禁止使用的致癌染料碱性红9(Basic red 9)和分散黄23(Disperse yellow 23)为模型分子,利用一步法快速制备的银纳米粒子为SERS基底并进行优化.通过... 详细信息

基于表面增强拉曼光谱(SERS)技术,发展了一种纺织品中染料定性检测的快速方法.以国家明确禁止使用的致癌染料碱性红9(Basic red 9)和分散黄23(Disperse yellow 23)为模型分子,利用一步法快速制备的银纳米粒子为SERS基底并进行优化.通过在纺织品表面直接滴加银纳米粒子的方法实现了纺织品中染料的快速SERS鉴别.研究结果表明,该方法不需要复杂的样品前处理过程,能够直接实现纺织品中染料的快速定性,且灵敏度高,对纺织品上两种禁用染料碱性红9和分散黄23的检测限分别为0.16和0.24 mg/kg,超出了国家标准的要求,有望成为一种实用的纺织品安全性评估技术.

关键词：表面增强拉曼光谱金属纳米粒子纺织品禁用染料快速检测

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电化学SPR协同催化对氯苯硫酚界面反应的SERS研究

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化学学报 2021年第12期79卷 1481-1485页

作者：袁宏宇徐敏敏姚建林苏州大学材料与化学化工学部苏州215123

表面等离激元共振(SPR)驱动的催化反应近年来广受关注,研究集中在SPR等外场作用下发生单一的界面催化反应生成新的物质,这对于表面反应设计和实现多步骤界面有机合成反应仍存在一定困难.本工作以对氯苯硫酚(4-CBT)为探针,利用表面增强... 详细信息

表面等离激元共振(SPR)驱动的催化反应近年来广受关注,研究集中在SPR等外场作用下发生单一的界面催化反应生成新的物质,这对于表面反应设计和实现多步骤界面有机合成反应仍存在一定困难.本工作以对氯苯硫酚(4-CBT)为探针,利用表面增强拉曼光谱(SERS)的极高表面灵敏度并结合金粒子单层膜(AuMLF)的玻碳电极(Au MLF@GC电极)作为基底在均匀性方面的优势,实现了电化学和SPR协同作用下界面催化反应及其过程的精准监测.结果表明,较负电位区间内,在光电协同催化作用下,4-CBT先发生脱氯反应生成苯硫酚(TP),然后4-CBT脱氯与偶联同时发生生成联苯-4,4’-二硫醇(4,4’-BPDT).提高激光功率可显著加快反应速率,且在中性溶液中反应速率最快.溴代苯硫酚以及邻位或间位二氯取代苯硫酚均可发生类似的脱卤素取代基和偶联反应,但邻位二氯取代物因空间位阻而导致偶联效率降低.

关键词：表面等离激元共振表面增强拉曼光谱电化学对氯苯硫酚偶联反应

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Au纳米粒子二聚体-Au片耦合体系“热点”的尺寸效应

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高等学校化学学报 2024年第6期45卷 130-137页

作者：曾自强张晨杰徐敏敏姚建林苏州大学材料与化学化工学部苏州215123

表面增强光谱“热点”效应一直是相关领域广受关注的主题,其中与尺寸和激发波长相关的动态“热点”转移效应的可控性是研究的重点和难点.本文利用有限元法(FEM)对Au纳米粒子球二聚体-Au片耦合体系进行了模拟计算,研究了激发波长和纳米... 详细信息

表面增强光谱“热点”效应一直是相关领域广受关注的主题,其中与尺寸和激发波长相关的动态“热点”转移效应的可控性是研究的重点和难点.本文利用有限元法(FEM)对Au纳米粒子球二聚体-Au片耦合体系进行了模拟计算,研究了激发波长和纳米粒子尺寸对体系不同间隙处电磁场增强的影响.结果表明,该体系所拥有的两种等离激元共振模式的分离和位置与纳米尺寸密切相关,并且影响该耦合体系的“热点”分布.当纳米粒子尺寸为30 nm,激发波长范围为450~535 nm和670~950 nm时,两种等离激元共振模式以协同效应为主,“热点”主要存在于粒子与粒子间隙;随着纳米粒子球尺寸增加至85~105 nm,激发波长范围分别为670~695nm和725~755 nm时,两种等离激元共振模式之间开始出现竞争效应,发现“热点”由粒子与粒子间隙处转移至粒子与金片间隙处.该研究结果为“热点”转移调控提供了新思路.

关键词： “热点” 表面等离极化激元金纳米粒子二聚体竞争效应转移效应

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PDMS-Au复合基底上多环芳烃分子的表面增强拉曼光谱

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高等学校化学学报 2017年第3期38卷 376-382页

作者：陈慧夏迪袁亚仙徐敏敏姚建林苏州大学材料与化学化工学部苏州215123

利用聚二甲基硅氧烷(PDMS)对有机物的富集功能,通过在金纳米粒子单层膜(Au MLF)表面旋涂薄层PDMS膜制备PDMS-Au MLF复合表面增强拉曼光谱(SERS)基底.研究了SERS增强性能与旋涂液浓度及稀释溶剂间的关系,考察了复合基底增强活性的均匀性... 详细信息

利用聚二甲基硅氧烷(PDMS)对有机物的富集功能,通过在金纳米粒子单层膜(Au MLF)表面旋涂薄层PDMS膜制备PDMS-Au MLF复合表面增强拉曼光谱(SERS)基底.研究了SERS增强性能与旋涂液浓度及稀释溶剂间的关系,考察了复合基底增强活性的均匀性.研究发现,采用叔丁醇为稀释溶剂,浓度为2%(质量分数)的旋涂液时所得复合基底表面多环芳烃(PAHs)的SERS信号强度最高,且此基底SERS信号强度偏差小于10%.分别以PDMS-Au MLF复合材料和Au MLF作为基底,对比研究了对萘、蒽、菲和芘4种多环芳烃的SERS检测能力.结果表明,PDMS-Au MLF复合基底对以上4种有机物的检出限分别为10^(-6),10^(-7),10^(-8)及10^(-7)mol/L,相比于单一Au MLF基底,其检测限至少降低了1个数量级,这主要源自于PDMS对PAHs的富集作用,且此类复合基底可用于多种多环芳烃混合物的特征识别.

关键词：表面增强拉曼光谱复合基底金多环芳烃聚二甲基硅氧烷

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