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National Science Review 2018年第5期5卷 694-702页

作者： Juanzhu Yan Jun Zhang Xumao Chen Sami Malola Bo Zhou Elli Selenius Xiaomin Zhang Peng Yuan Guocheng Deng Kunlong Liu Haifeng Su Boon K.Teo Hannu Hkkinen Lansun zheng nanfeng zheng state key laboratory for physical chemistry of solid surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Engineering Research Center for Nano-Preparation Technology of Fujian ProvinceCollege of Chemistry and Chemical EngineeringXiamen University School of Materials and Chemical Engineering Anhui Jianzhu University departments of Physics and chemistry Nanoscience CenterUniversity of Jyvskyl

Both the electronic and surface structures of metal nanomaterials play critical roles in determining their chemical properties. However, the non-molecular nature of conventional nanoparticles makes it extremely challenging to understand the molecular mechanism behind many of their unique electronic and surface properties. In this work, we report the synthesis, molecular and electronic structures of an atomically precise nanoparticle, [Ag206 L72]~q(L = thiolate, halide; q = charge). With a four-shell Ag7@Ag32@Ag77@Ag90 Ino-decahedral structure having a nearly perfect D5hsymmetry, the metal core of the nanoparticle is co-stabilized by 68 thiolate and 4 halide ligands. Both electrochemistry and plasmonic absorption reveal the metallic nature of the nanoparticles, which is explained by density functional theory ***, the nanoparticle can be considered as a superatom, just short of a major electron shell closing of 138 electrons(q = –4). More importantly, many of ligands capping on the nanoparticle are labile due to their low-coordination modes, leading to high surface reactivity for catalysing the synthesis of indoles from 2-ethynylaniline derivatives. The results exemplify the power of the atomic-precision nanocluster approach to catalysis in probing reaction mechanisms and in revealing the interplay of heterogeneous reactivities,electronic and surface structural dynamics, thereby providing ways for optimization.

关键词： metal nanoclusters atomically precise nanoparticles nobel metal superatom nanocatalysis

Molecular imaging of advanced atherosclerotic plaques with folate receptor-targeted 2D nanoprobes

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Nano Research 2020年第1期13卷 173-182页

作者： Zhide Guo Liu Yang Mei Chen Xuejun Wen Huanhuan Liu Jingchao Li Duo Xu Yuanyuan An Changrong Shi Jindian Li Xinhui Su Zijing Li Ting Liu Rongqiang Zhuang nanfeng zheng Haibo Zhu Xianzhong Zhang state key laboratory of Molecular Vaccinology and Molecular Diagnostics&Center for Molecular Imaging and Translational Medicine School of Public HealthXiamen UniversityXiamen361102China state key laboratory for Bioactive Substances and functions of Natural Medicines Beijing Key Laboratory of New Drug Mechanisms and Pharmacological Evaluation StudyInstitute of Materia MedicaChinese Academy of Medical Sciences&Peking Union Medical CollegeBeijing100050China College of Materials Science and Engineering Hunan UniversityChangsha410082China The state key laboratory for physical chemistry of solid surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryXiamen UniversityXiamen361005China Zhongshan Hospital Affiliated to Xiamen University Xiamen361004China

Vulnerable atherosclerotic plaques are responsible for most cardiovascular diseases(CVDs).folate receptor(fR)positive activated macrophages were thought to be a prominent component in the development of vulnerable *** objective of this study is to develop folate conjugated two-dimensional(2D)Pd@Au nanomaterials(Pd@Au-PEG-fA)for targeted multimodal imaging of the fRs in advanced atherosclerotic *** and imaging studies(single photon emission computed tomography(SPECT),computed tomography(CT)and photoacoustic(PA)imaging)were performed to confirm the prolonged blood half-life and enrichment of radioactivity in atherosclerotic *** signals were detected in vivo with SPECT,CT and PA imaging in heavy atherosclerotic plaques,which were significantly higher than those of the normal aortas after injection of Pd@*** studies with preinjection of excess fA could effectively reduce the targeting ability of Pd@Au-PEG-fA in atherosclerotic plaques,further demonstrating the specific binding of Pd@Au-PEG-fA for plaque *** characterization revealed that the signal of probe was in accordance with the high-risk *** summary,the Pd@Au-PEG-fA has favorable pharmacokinetic properties and provides a valuable approach for detecting high-risk plaques in the presence of fRs in atherosclerotic plaques.

关键词： 2D material folate receptor multifunctional imaging activated macrophages atherosclerosis

Hierarchical Homochiral Assembly of Polyhedral Cage-Type Nanoclusters

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CCS chemistry 2024年第10期6卷 2537-2548页

作者： Cheng-Long Deng Bao-Liang Han Ze-Yu Liu Zhong-Hua Pan Jiao He Yu-Long Li Zhi-Lin Yang Geng-Geng Luo Chen-Ho Tung Di Sun Lan-Sun zheng key laboratory of Environmentally friendly function Materials Ministry of EducationCollege of Materials Science and EngineeringHuaqiao UniversityXiamen 361021 School of chemistry and Chemical Engineering State Key Laboratory of Crystal MaterialsShandong UniversityJi’nan 250100 College of physical Science and Technology Xiamen UniversityXiamen 361005 College of chemistry and Environmental Engineering Sichuan University of Science and EngineeringZigong 643000 state key laboratory for physical chemistry of solid surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005

Hierarchical chiral self-assembly is of profound significance for biomolecules for their biological ***-precise metal nanoclusters(NCs)offer better opportunities to construct hierarchical ***,achieving hierarchical homochiral assembly of nanocrystals protected by achiral ligands has proven to be a formidable task,with existing examples primarily limited to heterochiral *** we put forward a hierarchical assembly strategy towards precisely fabricating highly ordered homochiral ***,clusterin-nanocage type copper-hydride NCs act as synthons,of which entity is featured with a hexagonal close-packed Cu_(9)kernel embedded in a C_(3)-symmetric trigonal-prismatic metallacage,leading to a chiral core-shell primary structure with either P or M *** four homochiral NCs combined with guests through synergistic noncovalent interactions spontaneously organize into a supramolecular tetrahedral secondary structure within a unit ***,these nanoscopic supramolecular motifs pack into tertiary hierarchical superlattice of chiral cubic crystalline ***,the crystalline material shows excellent robustness,and fascinating blueexcitable near-infrared thermally activated delayed fluorescence *** work not only exhibits that nanocage-type NCs can be smart as proteins to translate chiral primary structure into tertiary chiral hierarchical complexity,but also provides new insights into structure-to-superstructure,enabling bottom-up creation of higher-level hierarchical homochiral superlattice structures.

关键词： polyhydrido copper nanoclusters chiral polyhedral metallacage hierarchical homochiral assembly thermally activated delayed fluorescence

Cu_(2)O-SupportedAtomicallyDispersed Pd Catalysts for Semihydrogenation of Terminal Alkynes: Critical Role of Oxide Supports

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CCS chemistry 2019年第2期1卷 207-214页

作者： Kunlong Liu Ruixuan Qin Lingyun Zhou Pengxin Liu Qinghua Zhang Wentong Jing Pengpeng Ruan Lin Gu Gang fu nanfeng zheng Collaborative Innovation Center of chemistry for Energy Materials State Key Laboratory for Physical Chemistry of Solid Surfacesand Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Institute of Physics Chinese Academy of SciencesBeijing 100190China

Atomically dispersed catalysts have demonstrated superior catalytic performance in many chemical ***,limited success has been achieved in applying oxide-supported atomically dis-persed catalysts to semihydrogenation o... 详细信息

关键词： atomically dispersed catalyst support effect palladium semihydrogenation selective hydrogenation alkynes heterolytic activation of hydrogen galvanic displacement

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二维MoS_(2)纳米片的相工程

Science Bulletin 2023年第24期68卷 3084-3086页

作者：胡程奕郑南峰 state key laboratory for physical chemistry of solid surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand National&Local Joint Engineering Research Center for Preparation Technology of NanomaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation laboratory for Sciences and Technologies of Energy Materials of fujian Province(IKKEM) Xiamen 361102China

Phase engineering has been emerging as an effective strategy to tune the properties of two-dimensional transition-metal dichalcogenides(TMDs)for a variety of applications including electronics,catalysis,energy storage... 详细信息

关键词： catalysis separation transition

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金属纳米材料表面配体聚集效应

化学进展 2020年第8期32卷 1140-1157页

作者：秦瑞轩邓果诚郑南峰厦门大学化学化工学院固体表面物理化学国家重点实验室能源材料化学协同创新中心纳米材料制备技术国家地方联合工程研究中心厦门361005

金属纳米材料表面配体不仅可以稳定金属纳米颗粒,辅助合成特定尺寸和形貌的纳米材料,还可用于调控金属纳米颗粒的表面化学性质。由于现有表征技术的局限性,金属纳米材料表面有机配体的结构和功能一直以来并未被深入研究。得益于分子结... 详细信息

金属纳米材料表面配体不仅可以稳定金属纳米颗粒,辅助合成特定尺寸和形貌的纳米材料,还可用于调控金属纳米颗粒的表面化学性质。由于现有表征技术的局限性,金属纳米材料表面有机配体的结构和功能一直以来并未被深入研究。得益于分子结构明确金属纳米团簇和其他模型纳米材料体系的发展,配体在金属纳米材料表面的精确配位结构及其对催化过程的促进作用正不断被揭示出来。金属表面有机分子配位不仅可以调控表面金属电子结构,还可以分割表面原子周期性结构。表面有机配体的聚集可以进一步在金属表面构筑3D空间结构,改变纳米材料亲疏水性,并影响催化底物和反应中间体与表面的相互作用强弱和吸附构型。此外,有机配体与表面金属所组成的界面还可以构筑新的活性位点,改变催化反应路径,从而提升催化反应活性和选择性。金属纳米材料表面有机配体的聚集效应使得异相纳米材料可以同时表现出均相催化和酶催化的优势。

关键词：表界面配位化学金属纳米材料金属纳米团簇有机配体表面修饰表面聚集效应空间效应电子效应

包钯纳米颗粒的中空介孔硅铝酸盐纳米球的合成及其在多步催化反应和尺寸选择催化氢化中的应用(英文)

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化学学报 2013年第3期71卷 334-338页

作者：刘召辉方晓亮陈诚郑南峰厦门大学化学化工学院固体表面物理化学国家重点实验室 361005

最近,具有中空核壳结构的纳米材料在催化领域中有着深入的研究和广泛的应用.在本文中,我们使用一种简单易行的方法合成了一种包裹钯纳米颗粒的中空介孔硅铝酸盐纳米球(简写为Pd@HMAN).首先,通过一种先原位合成钯纳米粒子再对其进行二氧... 详细信息

最近,具有中空核壳结构的纳米材料在催化领域中有着深入的研究和广泛的应用.在本文中,我们使用一种简单易行的方法合成了一种包裹钯纳米颗粒的中空介孔硅铝酸盐纳米球(简写为Pd@HMAN).首先,通过一种先原位合成钯纳米粒子再对其进行二氧化硅包裹的方法,在Brij56-环己烷-水的反相胶束中合成了具有核壳结构的包裹钯纳米颗粒的二氧化硅纳米球(简写为Pd@SiO2).然后,使用CTAB,Na2CO3和NaAlO2试剂,通过简单的碱性条件下刻蚀Pd@SiO2的过程,我们成功得到了具有多孔性能的中空核壳型Pd@HMAN纳米催化剂.由于硅铝酸盐外壳具有酸催化作用,并且内核钯纳米颗粒又是一种高活性的催化媒介,因此,这种复合的多功能纳米催化剂能够很好的应用于多步催化反应中.此外,通过一个简单的热处理的方法,能够缩小硅铝酸盐外壳上的孔道,我们发现这种孔道调节后的Pd@HMAN纳米催化剂在尺寸选择性氢化反应中有很好的应用前景.

关键词：反相胶束核壳结构中空核壳结构钯多功能纳米催化剂尺寸选择性催化催化氢化

Rh/Al_(2)O_(3)催化剂在丙烷脱氢反应中的表面变化

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Chinese Journal of Catalysis 2024年第7期62卷 145-155页

作者：李书毅穆长乐何念秋徐杰郑燕萍陈明树厦门大学化学化工学院固体表面物理化学国家重点实验室福建厦门361005

丙烯是一种重要的化工原料,需求量较大且逐年增加.丙烷脱氢(PDH)是一种高效的生产丙烯过程,正逐步取代石脑油裂解成为重要的丙烯生产工艺.开发高效且稳定的PDH催化剂将对PDH工业发展起到积极的推动作用.Rh因其较好的C-H键活化能力,展现... 详细信息

丙烯是一种重要的化工原料,需求量较大且逐年增加.丙烷脱氢(PDH)是一种高效的生产丙烯过程,正逐步取代石脑油裂解成为重要的丙烯生产工艺.开发高效且稳定的PDH催化剂将对PDH工业发展起到积极的推动作用.Rh因其较好的C-H键活化能力,展现出作为PDH催化剂的巨大潜力,但关于Rh应用于PDH的报道较少.明确Rh物种尺寸对PDH产物选择性的影响,对后续设计高效且稳定的Rh基PDH催化剂至关重要.多相催化反应主要发生在催化剂的表面,因此,催化剂的表面状态对其催化性能具有重要的影响.在催化反应过程中,一些催化剂的表面状态会发生显著变化,这些变化会导致活性、产物选择性明显变化.通过采用(准)原位表面研究手段,能够清晰地了解催化剂在反应过程中的表面变化,这对于建立催化剂结构与反应性能之间的构效关系具有非常重要的意义.本文通过沉积-沉淀法制备了不同负载量的Rh/Al_(2)O_(3)催化剂,旨在探究Rh物种尺寸对PDH产物选择性的影响.球差电镜(AC-HAADf-STEM)观察显示,Rh物种以团簇和单原子的形式共存于Al_(2)O_(3)载体上.进一步通过准原位X射线光电子能谱(XPS)证实了不同化学态的Rh物种.通过固定床反应器对Rh/Al_(2)O_(3)催化剂的PDH性能进行测试,结果表明,催化剂在反应初始阶段需要经历诱导期.在此期间,甲烷的选择性显著降低,而丙烯的选择性显著升高,同时,丙烷的转化率显著降低.碳平衡计算表明,诱导期内产生了大量积碳.采用准原位XPS、低能离子散射谱(LEIS)和CO吸附红外光谱(CO-fTIR)研究了Rh/Al_(2)O_(3)催化剂在诱导期的表面变化.结果表明,在反应初始阶段,催化剂表面有大量积碳产生,这些积碳主要聚集在Rh物种表面,覆盖了Rh团簇,而Rh单原子则保持暴露状态,并作为PDH反应的活性中心.AC-HAADf-STEM结果表明,PDH反应4 h后,仍有Rh单原子存在于催化剂表面.结合Rh/Al_(2)O_(3)催化剂的PDH性能和准原位表征结果认为,丙烷在Rh团簇表面发生C-C键断裂反应,生成甲烷和积碳.积碳对Rh团簇的覆盖抑制了丙烷裂解反应,导致甲烷的选择性在诱导期显著降低;而Rh单原子则仍然暴露,具有催化PDH反应活性,并且是高选择性地生成丙烯的位点.该选择性的差异由丙烯在不同尺寸Rh物种上的吸附方式不同引起的,在Rh团簇表面以di-σ键吸附方式为主,吸附强度较强,丙烯不易脱附,并进一步发生裂解产生甲烷和积碳;而在Rh单原子上,丙烯以π键吸附方式存在,吸附强度较弱,不易发生副反应.对反应后的Rh/Al_(2)O_(3)催化剂进行分析,发现积碳主要为碳氢化合物和石墨碳,且随着反应进行,积碳从Rh团簇表面向Al_(2)O_(3)载体上转移.综上所述,本文通过使用准原位XPS,LEIS和CO-fTIR等技术探究了Rh/Al_(2)O_(3)催化剂在PDH反应中的表面变化,揭示了Rh物种尺寸对PDH产物选择性的影响.结果表明,Rh单原子对丙烯选择性有利,而在Rh团簇表面PDH产物主要为甲烷并产生积碳,同时积碳导致了催化剂在反应初始阶段的快速失活.本工作为后续高效Rh基PDH催化剂的设计提供参考.

关键词：丙烷脱氢铑积碳单原子准原位谱学表面变化

Enhancing sulfur cathode process via a functionalized complex molecule

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Nano Research 2023年第6期16卷 8385-8393页

作者： Qingyi zheng Xiaoxiang fan Guoqing Liu Qing Hou Jingmin fan Mingsen zheng Quanfeng Dong department of chemistry College of Chemistry and Chemical EngineeringCollaborative Innovation Centre of Chemistry for Energy Materials(iChEM)and State Key Laboratory of Physical Chemistry of Solid SurfacesXiamen UniversityXiamen 361005China

Lithium-sulfur batteries are regarded as promising next-generation energy storage batteries for their ultra-high theoretical energy ***,the complex sulfur electrode process with sluggish sulfur conversion reactions is a critical issue for lithiumsulfur batteries,in which catalytic interfacial reactions and accelerated lithium-ion diffusion are the key *** previous work has shown that implanting functional molecules with multiple redox properties in the electrode can break through the conventional diffusion layer constraints and achieve forced *** this work,a functionalized complex molecule,methylene blue anthraquinone-2-sulfonate(MB-AQ),with multiple redox activities as well as abundant active sites,was synthesized and introduced into the sulfur *** addition to accelerating the transport of lithium ions by reversible inhaling and exhaling lithium ions,the MB-AQ can combine polysulfides by its active sites to accelerate sulfur conversion *** from two functions of accelerating ion diffusion and catalyzing interfacial reactions,MB-AQ/reduced graphene oxide(rGO)/S cathode can achieve high initial capacities of 884 and 674 mAh·g^(−1)with stable cycling of 700 and 1,000 times at 1 and 4 C,*** is worth mentioning that the capacity of 462 mAh·g^(−1)can be achieved even at a high current density of 6 *** work provides a new approach to enhancing the sulfur cathode process.

关键词： lithium-sulfur batteries organic molecule dual-function sulfur conversion shuttle effect