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Interfacial oxidized Pd species dominate catalytic hydrogenation of polar unsaturated bonds

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Nano Research 2024年第1期17卷 228-234页

作者： Pengyao You Shaoqi Zhan Pengpeng Ruan Ruixuan Qin Shiguang Mo Yazhou Zhang Kunlong Liu Lansun zheng nanfeng zheng State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Department of Chemistry BMCUppsala UniversityBMC Box 576Uppsala S-75123Sweden Department of Chemistry University of OxfordOxford OX13QZUK

The determination of catalytically active sites is crucial for the design of efficient and stable catalysts toward desired ***,the complexity of supported noble metal catalysts has led to controversy over the locations of catalytically active sites(e.g.,metal,support,and metal/support interface).Here we develop a structurally controllable catalyst system(Pd/SBA-15)to reveal the catalytic active sites for the selective hydrogenation of ketones to alcohol using acetophenone hydrogenation as model *** investigations demonstrated that unsupported Pd nanocrystals have no catalytic activity for acetophenone ***,oxidized Pd species were catalytically highly active for acetophenone *** catalytic activity decreased with the decreased oxidation state of *** work provides insights into the hydrogenation mechanism of ketones but also other unsaturated compounds containing polar bonds,e.g.,nitrobenzene,N-benzylidene-benzylamine,and carbon dioxide.

关键词： oxidized Pd metal/oxide interface constant particle size Pd/SBA-15 acetophenone hydrogenation

Surface Ligand Evolution:Sulfur-Directed Covalent Bonding of PPh_(3) on Pd_(4)S with Improved Semi-hydrogenation of Terminal Alkynes

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Precision Chemistry 2024年第5期2卷 200-207页

作者： Wentong Jing Shiguang Mo Weijie Zhang Wenting Zhou Kunlong Liu Jie Wei Ruixuan Qin nanfeng zheng New Cornerstone Science Laboratory State Key Laboratory for Physical Chemistry of Solid SurfacesCollaborative Innovation Center of Chemistry for Energy Materialsand National&Local Joint Engineering Research Center of Preparation Technology of NanomaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China China Resources Cement Technology R&D(Guangxi)Co Ltd. Nanning 530008China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China

Surface modification of metallic nanocatalysts with organic ligands has emerged as an effective strategy to enhance catalytic selectivity,although offten at the expense of catalytic *** this study,we demonstrate a compelling approach by surface modifying Pd2S nanocrystals with PPhz ligands,resulting in a catalyst with excellent catalytic activity and durable selectivity for the semi-hydrogenation of terminal *** and theoretical investigations reveal that the presence of S sites on the Pd surface directs PPh_(3) ligands to preferentially form covalent bonds with S,creating distinctive surface S=PPh_(3) *** configuration induces a partial positive charge on Pd,facilitating hydrogen transfer and thus promoting catalytic ***,the covalent bond between the ligand and catalyst surface forms a robust network,ensuring ligand stability and increasing the hydrogenation energy barrier of ***,the Pd_(4)S@PPhz catalyst exhibits an improved catalytic selectivity with durability in terminal alkyne *** study introduces an effective strategy for designing selective hydrogenation catalysts with an enhanced performance.

关键词： Pd nanocatalysts surface modification selective hydrogenation catalytic stability alkyne semi-hydrogenation

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营造鼓励年轻学者解决真正科学问题的氛围

中国科学基金 2024年第3期38卷 543-544页

作者：郑南峰厦门大学嘉庚创新实验室厦门361005

2023年2月21日,中央政治局就加强基础研究进行集体学习,习近平总书记发表了重要讲话,要求推动基础研究实现高质量发展,这是前所未有的。近年来,我们也看到,国家自然科学基金委员会(以下简称“自然科学基金委”)围绕基础研究、应用基础... 详细信息

2023年2月21日,中央政治局就加强基础研究进行集体学习,习近平总书记发表了重要讲话,要求推动基础研究实现高质量发展,这是前所未有的。近年来,我们也看到,国家自然科学基金委员会(以下简称“自然科学基金委”)围绕基础研究、应用基础研究和人才培养,推动了多项重要改革措施落地落实。作为长期从事基础研究的一线科研人员,2016年以来本人陆续将自己的部分研究成果成功推向产业化,特别是近5年先后作为嘉庚创新实验室的常务副主任、主任参与到科研项目的管理与服务工作,对基础研究的重要性有了更全面的认识与理解,以下是我的几点看法。

关键词：科研人员科研项目创新实验室国家自然科学基金委员会人才培养应用基础研究集体学习管理与服务

Color center-rich γ-AlOpromotes propane dehydrogenation

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Science China Chemistry 2024年

作者： Yu Wang Xiang Wang Mengfei Qiao Qingyuan Wu Kunlong Liu Xiaodong Yi Ruixuan Qin Gang Fu nanfeng zheng State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Material SciencesZhejiang Normal University Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM)

The PtSn/Al2O3catalyst is commonly used in commercial propane dehydrogenation （PDH） processes,but it faces challenges in the deactivation and periodic regeneration due to metal aggregation and coke deposition at high *** Al3+pentahas been proven to be beneficial for enhancing catalytic stability,bottom-up synthesis protocols usually restrict their ***,a facile post-treatment approach using acetic acid was applied to create color centers （electrons trapped within oxygen vacancies） on γ-Al3+***,the content of Alpentawas enriched to 18.3%.Then,the pre-established PtSn clusters were *** electrons facilitated the formation of ultrafine PtSn nanoparticles （～2 nm）,and the Al3+pentasites prevented the sintering of PtSn by constructing the strong Al3+penta–O–Sn ***,the catalytic durability of the catalyst prepared by conventional impregnation methods was remarkably extended from 186 h for the color center-free sample to 1,000 h using the HAc–*** facile post-modification was further successfully extended to commercial Al2O3pellets without altering their mechanical properties,highlighting its potential in industrial applications.

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Coordination chemistry of atomically dispersed catalysts

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National Science Review 2018年第5期5卷 636-638页

作者： Pengxin Liu nanfeng zheng Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory for Physical Chemistry of Solid SurfacesandDepartment of ChemistryCollege of Chemistry and Chemical EngineeringXiamen University

The last decade has witnessed the rapid development of atomically dispersed catalysts. With every active metal atom anchored on the surface of supports,atomically dispersed catalysts offer the maximum atom efficiency, helping to create cost-effective catalysts, particularly those based on earth-scarce *** it is still in intense debate whether single metal atoms can provide better catalytic activities than surface atoms of metal nanoparticles, an increasing

关键词： TiO

Amine facilitates the synthesis of silica-supported ultrasmall bimetallic nanoparticles

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Science China Materials 2018年第8期61卷 1129-1131页

作者： nanfeng zheng Pengxin Liu Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory for Physical Chemistry of Solid Surfaces and Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University

Supported catalysts based on metal nanoparticles are a class of widely used heterogeneous catalysts in *** catalytic performances of supported metal catalysts are highly determined by many parameters of metal nanopart... 详细信息

关键词： Amine facilitates the synthesis of silica-supported ultrasmall bimetallic nanoparticles

Multifunctional ultrasmall Pd nanosheets for enhanced near-infrared photothermal therapy and chemotherapy of cancer

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Nano Research 2015年第1期8卷 165-174页

作者： Shaoheng Tang Mei Chen nanfeng zheng State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials andDepartment of Chemis try College of Chemistry and Chemical Engineering Xiamen University Xiamen Fujian 361005 China

Near-infrared （NIR） photothermal therapy has developed very quickly in recent years. However, its clinical applications are hindered by many practical problems, such as low accumulation in tumors, high laser power density and high biotoxicity in vivo. Herein, a versatile system combining chemotherapy with photothermal therapy for cancer therapy using ultrasmall Pd nanosheets （SPNS） has been developed. The SPNS can serve as pH-responsive drug carriers to efficiently deliver DOX into cancer cells and tumors. On the other hand, the coordinative loading of DOX on SPNS enhances its accumulation in tumor tissue. So we can efficiently ablate tumor using low-intensity laser radiation. Importantly, with ultrasmall size （-4.4 nm）, SPNS surface-functionalized with reduced glutathione （GSH） can be cleared from the body through the renal system into the urine. This cancer therapeutic nanosystem, which exhibits a significant synergistic effect and low systemic toxicity, has great potential for clinical applications.

关键词： photothermal therapy chemotherapy Pd nanosheets drug delivery synergistic effect

Special topic on strategies for developing energy-related physical chemistry

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Science China Chemistry 2017年第11期60卷 1377-1378页

作者： Zhong-Qun Tian 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

Increasing global energy demand and environment issue have pushed us to develop technologies for efficient utiliza- tion of fossil fuels and also seek for renewable energy re- sources. Chemistry plays a crucial role in the acquisition, generation, distribution, and utilization of energy in differ- ent forms although it is not the only contributing subject. Currently, fossil fuels are the primary source to provide the majority of the world＇s energy. While the efficient utiliza- tion of fossil fuels requires deep understanding of the ener- gy transformation processes associated with the breaking and reorganization of chemical bonds, the use of many re- newable energy resources often involves chemical trans- formations with electron transfer. For these reasons, energy chemistry has been recently emerging as a new interdisci- plinary area to address chemistry issues associated with energy technologies.

关键词：可再生能源化学战专题物理化石燃料高效利用重组技术环境问题

Two-dimensional Pd-based nanomaterials for bioapplications

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Science Bulletin 2017年第8期62卷 579-588页

作者： Xiaolan Chen Saige Shi Jingping wei Mei Chen nanfeng zheng State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials and Engineering Research Center for Nano-Preparation Technology of Fujian Province College of Chemistry and Chemical Engineering Xiarnen University Xiarnen 361005 China

Noble metal nanomaterials have been extensively explored in cancer diagnostic and therapeutic applica- tions owing to their unique physical and chemical properties, such as facile synthesis, straightforward surface functionalization, strong photothermal effect, and excellent biocompatibility. Herein, we summa- rize the recent development of two-dimensional （2D） Pd-based nanomaterials and their applications in cancer diagnosis and therapy. Different synthetic strategies for Pd nanosheets and the related nanostruc- tures, including Pd@Au, Pd@Ag nanoplates and mesocrystalline Pd nanocomlla, are first discussed. Together with their unique properties, the potential bioapplications of these 2D Pd nanomaterials are then demonstrated. With strong absorption in near-infrared （NIR） region, these nanomaterials have great potentials in cancer photothermal therapy （PTr）. They also readily act as contrast agents in photoacoustic （PA） imaging or X-ray computed tomography （CT） to achieve image-guided cancer therapy. Moreover, significant efforts have been devoted to studying the combination of PTr and other treatment modalities （e.g., chemotherapy or photodynamic therapy） based on Pd nanomaterials. The remarkable synergistic or collaborative effects to achieve better therapeutic efficacy are discussed as well. Additionally, the biosaf- ety of 2D Pd-based nanomaterials in vitro and in vivo was evaluated. Finally, challenges for the applica- tions of Pd-based nanomaterials in cancer diagnosis and therapy, and future research prospects are highlighted.

关键词： 2D nanomaterials Palladium Optical properties Bioimaging Photothermal therapy Combination therapy