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Special Column on Nanoparticles/MOFs Synergistic Catalysis

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Chemical Research in Chinese Universities 2022年第6期38卷 I0001-I0002页

作者： OUYANG Junchen zhang suoying HUO Fengwei Nanjing Tech University Nanjing 211816P.R.China

Synergistic catalysis,which utilizes at least two different catalysts or a multi-component catalyst to facilitatechemical reactions,has been regarded as a classic strategy for catalyst design and catalytic *** the explosive development of new materials in the last two decades,new synergistic catalysts with previously unattainable catalytic performance and synergistic effects have sprung up.

关键词： synergistic catalyst utilize

Synergistic Catalysis of Enzymes and Biomimetic MOFs: Immobilizing Cyt c on Two-dimensional MOFs to Enhance the Performance of Peroxidase

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Chemical Research in Chinese Universities 2022年第6期38卷 1356-1360页

作者： WANG Yitong MENG Fanchen SU Ruifa SUN Changrui HAN Qianqian zhang Weina zhang suoying Key Laboratory of Flexible Electronics(KLOFE) Institute of Advanced Materials(IAM)Nanjing Tech UniversityNanjing 211816P.R.China

Metal-organic frameworks(MOFs) have been widely regarded as promising carriers for enzyme immobilization owing to their advantages in improving loading and regulating interaction with enzymes. However, they are still suffering from the problems of slow mass transfer and compromising activity. In this paper, the active two-dimensional(2D) MOF of Cu-TCPP(Fe)[TCPP=tetrakis(4-carboxy-phenyl)porphyrin], which possesses the biomimetic architecture of peroxidase, was adopted to anchor cytochrome(Cyt c) for the enhancement of catalytic activity. The atomic/nanometer thickness and micrometer lateral dimension of 2D MOFs can ensure the full exposure of immobilized enzymes and a shorter diffusion distance for the reactant molecules. Besides, the active carrier can provide synergistic catalysis and activity compensation during the reaction. When tested in the decomposition reaction of H_(2)O_(2), Cyt c/Cu-TCPP(Fe) exhibited nearly twice catalytic activity and an accelerated catalytic rate compared to free Cyt c.

关键词： Enzyme immobilization 2D metal-organic framework Biomimetic catalyst Catalysis

Highly active and stable Co nanoparticles embedded in nitrogen-doped mesoporous carbon nanofibers for aqueous-phase levulinic acid hydrogenation

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Green Energy & Environment 2021年第4期6卷 567-577页

作者： Shuai Shao Ying Yang Shangwei Guo Shijie Hao Feng Yang suoying zhang Yang Ren Yangchuan Ke State Key Laboratory of Heavy Oil Processing China University of PetroleumChangpingBeijing102249China X-Ray Science Division Argonne National Laboratory9700 S.Cass Ave.ArgonneIllinois60439USA

Developing a highly active and durable non-noble metal catalyst for aqueous-phase levulinic acid(LA)hydrogenation to g-valerolactone(GVL)is an appealing yet challenging ***,we report well-dispersed Co nanoparticles(NPs)embedded in nitrogen-doped mesoporous carbon nanofibers as an efficient catalyst for aqueous-phase LA hydrogenation to *** Co zeolitic imidazolate framework(ZIF-67)nanocrystals were anchored on the sodium dodecyl sulfate modified wipe fiber(WF-S),yielding one-dimensional(1-D)structured composite(ZIF-67/WF-S).Subsequently,Co NPs were uniformly embedded in nitrogen-doped mesoporous carbon nanofibers(Co^(R)NC/SMCNF)through a pyrolysis-reduction strategy using ZIF-67/WF-S as the *** from introducing modified wipe fiber WF-S to enhance the dispersion of Co NPs,and Co^(0) with Co-N_xdual active sites,the resulting Co^(R)NC/SMCNF catalyst shows brilliant catalytic activity(206 h^(-1) turnover frequency).Additionally,the strong metal-support interactions greatly inhibited the Co NPs from aggregation and leaching from the mesoporous carbon nanofibers,and thus increasing the reusability of the Co^(R)NC/SMCNF catalyst(reusable nine times without notable activity loss).

关键词： Co nanoparticles Mesoporous carbon nanofiber Dual active sites Aqueous levulinic acid hydrogenation High stability

Incorporating metal nanoparticles in porous materials via selective heating effect using microwave

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Nano Research 2024年第4期17卷 3175-3179页

作者： Yingyu Zhou Jiacheng Liu Fuyuan Sun Junchen Ouyang Ruifa Su Fanchen Meng Yongqi Luo Cheng Xu Weina zhang suoying zhang Fengwei Huo Key Laboratory of Flexible Electronics(KLOFE)&Institute of Advanced Materials(IAM) Nanjing Tech UniversityNanjing 211816China

Metal nanoparticle@porous material composites have attracted increasing attention due to their excellent synergistic catalytic ***,it is a challenge to introduce metal nanoparticles into cavities of porous materials without agglomeration on the *** the progress achieved,a universal approach that can integrate different kinds of metal nanoparticles and porous materials is still highly *** we report a facile and general approach to fabricating metal nanoparticle@porous materials by microwave-triggered selective *** microwave can pass through the non-polar solvent and act on the polar solvent in the porous materials,causing the polar solvent to be heated,vaporized,and away from the pores of porous *** local void produced by the escape of polar solvent facilitates non-polar solvent containing metallic precursor to be dragged into the narrow pores,followed by further reduction,resulting in the complete encapsulation of nanoparticles.A series of metal nanoparticles@porous materials,ranging from metal-organic frameworks(MOFs)to zeolites,are successfully prepared by this method and show excellent size selectivity in catalytic reactions.

关键词： porous material nanoparticle encapsulation microwave synthesis selective heating effect selective catalysis

Chemo-Biocascade Reactions Enabled by Metal-Organic Framework Micro-Nanoreactor

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Research 2023年第1期2022卷 15-25页

作者： Jing zhang Yu Shen Na Jin Xiaopeng Zhao Hongfeng Li Ning Ji Yingjie Li Baoli Zha Lin Li Xikuang Yao suoying zhang Fengwei Huo Weina zhang Key Laboratory of Flexible Electronics(KLOFE) Institute of Advanced Materials(IAM)Nanjing Tech University(NanjingTech)Nanjing 211800China The Institute of Flexible Electronics(IFE Future Technologies)Xiamen UniversityXiamen361005 FujianChina

The one-pot combination of biocatalytic and chemocatalytic reactions represents an economically and ecologically attractive concept in the emerging cascade processes for *** mutual incompatibility of biocatalysis and chemocatalysis,however,usually causes the deactivation of catalysts,the mismatching of reaction dynamic,and further challenges their integration into concurrent ***,we have developed a convenient strategy to construct versatile functional metal-organic framework micro-nanoreactors(MOF-MNRs),which can realize not only the encapsulation and protection of biocatalysts but also the controllable transmission of substances and the mutual communication of the incompatible ***,the MOFs serving as the shell of MNRs have the capability of enriching the chemocatalysts on the surface and improving the activity of the chemocatalysts to sufficiently match the optimum aqueous reaction system of biocatalysts,which greatly increase the efficiency in the combined concurrent *** strategy of constructing MOF-MNRs provides a unique platform for connecting the“two worlds”of chemocatalysis and biocatalysis.

关键词： catalysis mutual connecting

CO_(2) coordination-driven top-down synthesis of a 2D non-layered metal-organic framework

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Fundamental Research 2022年第5期2卷 674-681页

作者： Yannan Zhou Pengfei Yan suoying zhang Yunxiao zhang Hongwei Chang Xiaoli Zheng Jingyun Jiang Qun Xu College of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450052China Henan Institute of advanced technology Zhengzhou UniversityZhengzhou 450052China Key Laboratory of Flexible Electronics&Institute of Advanced Materials Nanjing Tech University30 South Puzhu RoadNanjing 211816China

Combining the physical advantages of two-dimensional(2D)inorganic nanosheets and the modular design and programmed structure of metal-organic frameworks(MOFs),2D MOFs remain at the forefront of functional material *** tremendous efforts,precise control in the synthesis of 2D nonlayered MOFs with predesigned topology for desired applications remains *** in the bottom-up synthesis of 2D nonlayered MOFs via ligand exchange motivated us to incorporate partial BTC(BTC=1,3,5-benzenetricarboxylate)ligand dissociation and CO_(2) capped coordination into the top-down treatment of bulk Cu-BTC MOF,leading to successful conversion of a 3D nonlayered network to a 2D Cu-based topological ***,a supercritical CO_(2)-containing solvent mixture is employed to provide the desired defect and coordination ***,our work introduces a new top-down concept based on modulated synthesis to fabricate high-quality 2D nonlayered MOFs for the first time.

关键词： Top-down Metal-organic frameworks 2D nonlayered Cu-BTC CO_(2)coordination Defect engineering

Solar Energy for Value-Added Chemical Production by LightPowered Microbial Factories

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CCS Chemistry 2024年第7期6卷 1776-1788页

作者： Haibo Wu Xilong Feng Liangjun Wang Cheng Chen Peng Wu Linpo Li Jinjie Xu Fan Qi suoying zhang Fengwei Huo Weina zhang Key Laboratory of Flexible Electronics(KLOFE) Institute of Advanced Materials(IAM)School of Flexible Electronics(Future Technologies)Nanjing Tech University(NanjingTech)Nanjing 211816

The light-driven material-microorganism biohybrid system has the potential to transfer solar energy for chemical ***,few studies have reported the construction of biohybrid systems using light-responsive materials with nonmodel strains that have been widely used in practical industrial production for value-added chemicals,especially with regard to the mechanism of action of photogenerated charges in the cytoplasm,probably due to the complexity of their anabolic ***,a biohybrid system as a research mode was constructed by electrostatically self-assembling a highly efficient light-harvesting material of graphite-phase nitrided carbon(g-C_(3)N_(4))nanosheets with nonmodel strains(Phaffia rhodozyma)for synthesis of nutritional chemical *** biohybrid interface enabled efficient separation,transfer,and transport of photogenerated charges from g-C_(3)N_(4) into the interior of ***,which improved the substance metabolism and the energy metabolism of ***,photogenerated charges can significantly promote the accumulation of precursors along the astaxanthin anabolic pathway and enhance the cytoplasmic redox environment and ATP levels in the interior of ***,even under adverse conditions(such as enzyme inhibitors),thus increasing the yield of astaxanthin compared to the traditional culture of *** study not only provides new ideas for converting solar energy into value-added chemicals,but it also provides guidance for regulating microbial synthesis plants.

关键词： biohybrid system light-driven graphitephase nitrided carbon Phaffia rhodozyma astaxanthin

MOF作模板制备多孔Au/Cu_xO催化剂及其CO氧化性能

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化工学报 2016年第6期67卷 2325-2331页

作者：刘朋飞张所瀛杨祝红陆小华南京工业大学化学化工学院材料化学工程国家重点实验室江苏南京210009

采用MOF材料作模板,通过在Cu-BTC材料表面预先负载贵金属Au再热解的方法,成功制备了具有正八面体结构的新型多孔Au/Cu_xO负载型催化剂。通过降低热解环境中的O_2浓度,调节氧化时间,实现了Au/Cu-BTC氧化产物组分的调节,分别制得了Au/Cu_2... 详细信息

采用MOF材料作模板,通过在Cu-BTC材料表面预先负载贵金属Au再热解的方法,成功制备了具有正八面体结构的新型多孔Au/Cu_xO负载型催化剂。通过降低热解环境中的O_2浓度,调节氧化时间,实现了Au/Cu-BTC氧化产物组分的调节,分别制得了Au/Cu_2O、Au/Cu_2O-Cu O、Au/CuO复合催化材料。将其用于CO催化氧化,发现所有Au/Cu_xO催化剂都表现出比Cu-BTC和Au/Cu-BTC更优异的催化性能,其中由于拥有较高的比表面积、Cu_2O含量以及更好的Au的分散性,Au/Cu_2O的CO氧化活性最佳,180℃即能实现CO的完全转化。

关键词：金属-有机骨架材料催化剂纳米结构多孔材料 Cu-BTC Au/Cu2O

层层沉积热处理法制备超薄Cu3(BTC)2膜

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化工学报 2013年第11期64卷 4255-4261页

作者：仇龙云李力成冯新付双钦张所瀛陆小华杨祝红南京工业大学化学化工学院、材料化学工程国家重点实验室江苏南京210009

基于层层沉积法,引入简单易控的热处理方式在玻璃基底表面制备出高结晶度且致密无裂缝的Cu3(BTC)2膜,并详细探讨热处理温度、组装时间和组装溶剂对Cu3(BTC)2成膜的影响。FESEM分析结果显示:膜层的厚度仅为200nm;热处理有利于获得完整的... 详细信息

基于层层沉积法,引入简单易控的热处理方式在玻璃基底表面制备出高结晶度且致密无裂缝的Cu3(BTC)2膜,并详细探讨热处理温度、组装时间和组装溶剂对Cu3(BTC)2成膜的影响。FESEM分析结果显示:膜层的厚度仅为200nm;热处理有利于获得完整的晶体结构,且高温下膜层不会产生裂纹;组装时间为5min或10min,Cu3(BTC)2颗粒尺寸小且均一。然而,当组装时间延长至20min,尺寸变得不均一,膜层表面变粗糙;通过改变组装溶剂环境,可以制备出不同维数的晶体膜。

关键词：金属有机骨架材料 Cu3(BTC)2 膜层层沉积法热处理表面聚合物