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large-scale synthesis of low-cost 2D metal–organic frameworks for highly selective photocatalytic CO_(2)reduction

Nano Research 2023年第5期16卷 7756-7760页

作者： Ning-Yu Huang Zhen-Yu Chen Fei-Long Hu Chun-Yan Shang Wenjuan Wang Jia-Run Huang Chuan Zhou Lei Li Qiang Xu Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials(SKLPM) Southern University of Science and TechnologyShenzhen 518055China Department of Chemistry Southern University of Science and TechnologyShenzhen 518055China Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055China SUSTech-Kyoto University Advanced Energy Materials Joint Innovation Laboratory(SKAEM-JIL) Southern University of Science and TechnologyShenzhen 518055China Key University Laboratory of Highly Efficient Utilization of Solar Energy and Sustainable Development of Guangdong Southern University of Science and TechnologyShenzhen 518055China MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-sen UniversityGuangzhou 510275China

Two-dimensional metal–organic frameworks(2D MOFs),as a new type of 2D materials,have been widely applied in various applications because of their unique structures and exposed active ***,we reported two low-cost 2D MOFs constructed by a raw chemical succinic acid(SA),M-SA(M=Ni or Co),which served as efficient photocatalysts for the reduction of CO_(2)to *** advantage of the thinness and open metal sites,the ultrathin Ni-SA nanosheets(ca.3.6 nm)exhibited excellent CO production of 6.96(7)mmol·g^(−1)·h^(−1)and CO selectivity of 96.6%.Photoelectrochemical tests and theoretical calculations further confirmed the higher charge transfer efficiency and unsaturated metal sites for promoting photocatalytic *** importantly,Ni-SA can also be synthesized in large-scale by an energy-saving method under room temperature,strongly suggesting its promising future and potential for practical applications.

关键词： two-dimensional metal–organic framework low-cost photocatalysis CO_(2)reduction large-scale synthesis

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large-scale synthesis of lithium-and manganese-rich materials with uniform thin-film Al2O3 coating for stable cathode cycling

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Science China Materials 2020年第9期63卷 1683-1692页

作者： Yuqiong Kang Zheng Liang Yun Zhao Haiping Xu Kun Qian Xiangming He Tao Li Jiangang Li School of Chemical Engineering Beijing Institute of Petrochemical TechnologyBeijing 102617China Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology Beijing 102617China State Key Laboratory of Automotive Safety and Energy Tsinghua UniversityBeijing 100084China Department of Chemistry and Biochemistry Northern Illinois UniversityDeKalbIL 60115USA Materials Sciences Division Lawrence Berkeley National LaboratoryBerkeleyCA 94720USA

The lithium-and manganese-rich layered oxide(LMR)holds great promise as a cathode material for lithiumion battery(LIB)applications due to its high capacity,high voltage and low ***,its poor initial Coulombic efficiency(ICE)and unstable electrode/electrolyte interface with continuous growth of the solid electrolyte interphase leads to high impedance and large *** effects cause severe capacity loss and safety *** this work,we have developed a novel approach to fabricate a stable LMR cathode with a uniform thin layer of aluminum oxide(Al2O3)coated on the surface of the LMR *** synthesis approach uses the microemulsion method that is environment-friendly,cost-effective and can be easily ***,an 8-nm layer of Al2O3 is shown to be effective in stabilizing the electrode/electrolyte interface(enhanced ICE to82.0%and moderate impedance increase over 200 cycles).Moreover,the phase transformation from layered to spinel is inhibited(96.3%average voltage retention)and thermal stability of the structure is significantly increased(heat release reduced by 72.4%).This study opens up a new avenue to address interface issues in LIB cathodes and prompts the practical applications of high capacity and voltage materials for high energy density batteries.

关键词： lithium ion batteries lithium-and manganese-rich layered oxides surface modification metal oxide thin film uniform coating large-scale synthesis battery safety

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Monodisperse Fe3O4 spheres: large-scale controlled synthesis in the absence of surfactants and chemical kinetic process

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Science China Materials 2019年第10期62卷 1488-1495页

作者： Yana Li Zhiyi Wang Zeeshan Ali Kesong Tian Junjie Xu Wei Li Yanglong Hou Beijing Key Laboratory for Magnetoelectric Materials and Device(BKLMMD) Beijing Innovation Center for Engineering Science and Advanced Technology(BIC-ESAT)Department of Materials Science and EngineeringCollege of EngineeringPeking UniversityBeijing 100871China

Fe3 O4 has attracted tremendous interest in vast areas of biomedicine and catalysis as well as environment ***,it is highly desired to fully understand the chemical kinetic process and propose a general,surfactantfree,large-scale synthesis approach for Fe3 O4 ***,we developed a facile scalable solvothermal method in the absence of surfactants to produce Fe3 O4 spheres with the yield of 5.1 g,which present tunable sizes from 107 to 450 nm by modulated molar ratio of Fe3+/COO-in the ***,it is observed that the reactants undergo a redox process,composed of a precipitation-dissolution equilibrium combined with a coordination reaction(termed as RPC),to the final product based on the LaMer *** is worth noting that the generation of di-carboxyl group and its coordination with iron cations determine the formation of Fe3 O4 *** work not only offers a strategy to precisely tailor the particle size in scalable synthesis process,but also gives the insight on the role of dihydric alcohol in the formation mechanism of Fe3 O4 spheres in the absence of surfactants.

关键词： Fe3O4spheres surfactant-free large-scale synthesis chemical kinetic process

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Cobalt phosphide nanoparticles supported within network of N-doped carbon nanotubes as a multifunctional and scalable electrocatalyst for water splitting

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Journal of Energy Chemistry 2021年第1期30卷 130-138,I0005页

作者： Dongxu Yang Wenqiang Hou Yingjiong Lu Wanli Zhang Yuanfu Chen School of Electronic Science and Engineering and State Key Laboratory of Electronic Thin Films and Integrated DevicesUniversity of Electronic Science and Technology of ChinaChengdu 610054SichuanChina Department of Physics School of Scienceand Everest Research InstituteTibet UniversityLhasa 850000Xizang(Tibet)Autonomous RegionChina School of Electronic Science and Engineering Xi’an Jiaotong UniversityXi’an 710049ShaanxiChina

In order to realize industrial production of hydrogen through water splitting,it is essential to develop a cost-efficient and scalable approach to synthesize nonprecious electrocatalysts with sufficiently high activity and stability to replace commercial noble-metal-based *** we synthesize cobalt phosphide nanoparticles dispersed within nitrogen-doped carbon nanotube network(CP@NCNT) via scalable spray drying and thermal *** a multifunctional electrocatalyst,the CP@NCNT hybrid delivers outstanding activity for HER(in both acidic and alkaline electrolytes),OER and overall water ***,it shows an ultra-low overpotental of 94 mV to obtain 10 mA cm-2 in *** also demonstrates outstanding activity in overall water splitting,requiring only 1.619 V to deliver 10 mA cm-2with more than 72 h’ long-term *** combination of notable performance,multi-functionality and highly scalable spray-drying synthesis method enables this material as a novel and cost-efficient transition metal-based electrocatalysts for overall water splitting.

关键词： Obalt phosphides Carbon nanotube Nitrogen doping large-scale synthesis Overall water splitting

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Protonic recognition and assembly for the creation of porous Bronsted acid catalysts with enhanced catalytic efficiency

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Chinese Chemical Letters 2023年第8期34卷 158-161页

作者： Liping Huang Mingyun Liang Yajun Fang Jehan Kim Yuntian Yang Zhegang Huang PCFM LIFM LabSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275China Guangdong Provincial Key Laboratory of Optical Chemicals Xinhuayue GroupMaoming 525000China Shenzhen Grubbs Institute Department of ChemistrySouthern University of Science and TechnologyShenzhen 518055China Pohang Accelerator Laboratory PostechPohangGyeongbukKorea

Due to the high local concentration of substrates in confined space, porous solid Bronsted acids have been extensively explored for efficient acid-catalyzed reaction. However, the porous structures with strong Bronsted acids lack long-term stability due to chemical hydrolysis. Moreover, the products inhibition effect in confined rigid cavities severely obstructs subsequent catalysis. Here, tubular Bronsted acid catalyst with unique recognition of protons was presented by self-assembly of p H-responsive aromatic amphiphiles. The responsive assembly could mechanically transfer hydrogen ions from low-concentration acidic solution into tubular defined pores, thereby producing effective catalytic activity for Mannich reactions in mildly acidic solution. Notably, the tubular catalyst unfolded into flat sheets upon addition of triethylamine for efficient release of products, which could be recovered by subsequent acidification and the catalytic activity still remained. Therefore, the porous Bronsted acid with reversible assembly provides a new strategy for mass synthesis through increasing conversion times.

关键词： Tubular Brosted acid Protonic recognition Dynamic assembly Heterogeneous catalysis large-scale synthesis

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A nano-liter droplet-based microfluidic reactor serves as continuous large-scale production of inorganic perovskite nanocrystals

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Science China Materials 2022年第10期65卷 2746-2754页

作者： Yuhao Geng Jiazhuang Guo Si Da Ling Xingjiang Wu Hengyuan Liu Zhuo Chen Su Chen Jianhong Xu The State Key Laboratory of Chemical Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical Engineering and Jiangsu Key Laboratory of Fine Chemicals and Functional Polymer MaterialsNanjing Tech UniversityNanjing 210009China

Lead halide perovskite nanocrystals(NCs)exhibit high photoluminescence quantum yield(PLQY),high defect tolerance,narrow half peak width,and wide luminous gamut,making them the ideal optoelectronic materials in numerous ***,their production still suffers from the limited productivity at the bench *** this work,we fabricated CsPbX3(X=Cl,Br,I)NCs within droplet-based micro-reactors,where both the nucleation and growth processes could be precisely controlled inside 130-nL *** provides a new paradigm for the large-scale synthesis of perovskite NCs with high *** with other synthetic methods,this method can increase the concentration of reactant precursors by 3±116 times,while lowering the ligand to reactant ratio to 2%±50%of the commonly used hot-injection *** modulating the reaction temperature and residence time,the structure-function relationship between the morphology of NCs and PL properties was extensively *** microfluidic-based process allows the flexible adjustment in the proportion of PbX2 precursors to achieve the fabrication of perovskite NCs whose luminescence range covers the entire visible spectrum(406±677 nm)within one ***,perovskite NCs with different halide ions were encapsulated in polymethyl methacrylate to prepare a colored light-emitting diode strip.

关键词： perovskite nanocrystals microfluidic method droplet-based microreactor large-scale synthesis online regulation

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