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CCS Chemistry 2022年第4期4卷 1376-1385页

作者： Hao Lv Fang Lv Huaiyu Qin Xiaowen Min Lizhi Sun Na Han Dongdong Xu Yanguang Li Ben Liu College of Chemistry Sichuan UniversityChengdu 610064 Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123 Jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Center of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023

Mesoporous single crystals have unique potential in catalysis,but remain unexplored owing to the enormous synthetic challenge that they ***,we report a facile soft-template method to prepare palladium(Pd)and Pd alloy nanocubes with single-crystallinity and abundant *** successful formation of these exotic nanostructures essentially relies on the cointroduction of cetyltrimethylammonium chloride as the surfactant template and extra Cl^(−) ions as the facet-selective capping agent under well controlled experimental *** to their large surface areas and penetrating mesoporous channels,our products exhibit a great performance for electrochemical CO_(2) *** best sample from alloying palladium with copper enables the efficient formate production with high selectivity(90∼100%)over a broad potential range,and great stability even under the working potential as cathodic as −0.5 V versus a reversible hydrogen *** performance metrics are far superior to previous Pd-based materials,and underscore the structural advantages of our products.

关键词： single-crystalline mesoporous palladium electrochemical CO_(2)reduction stability

Effect of particle size of single-crystalline hierarchical ZSM-5 on its surface mass transfer in n-heptane catalytic cracking

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Chinese Journal of Chemical Engineering 2023年第11期63卷 148-157页

作者： Xiaoxue Zhang Shuman Xu Jing Hao Xiaojin Xie Fengqiu Chen Dangguo Cheng College of Chemical and Biological Engineering Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture TechnologyZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China

single-crystalline hierarchical ZSM-5 zeolites with different particle sizes(namely 100,140,and 200 nm)were successfully prepared by adjusting the amount of tetrapropylammonium hydroxide(TPAOH),and investigated in n-heptane catalytic cracking *** measurements by zero-length column(ZLC)method showed that the apparent diffusivities of n-heptane decreased with the reduction of particle size,indicating the existence of surface ***,with the decrease of particle size,the additional diffusion path length increased,which meant the influence of surface barriers became more *** the change of surface barriers,the intracrystalline diffusion still dominated the overall *** performance showed that the zeolite with smaller particle size had better stability.

关键词： single-crystalline Hierarchical ZSM-5 Particle size Surface barriers n-Heptane catalytic cracking

Boosting electrocatalytic hydrazine oxidation at single-crystalline Ni nanosheets with embedded NiZn

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Progress in Natural Science:Materials International 2023年第5期33卷 710-717页

作者： Xia Wei Hongbin Dai Chuangwei Liu Song Li School of Material Science and Engineering Northeastern University

Hydrazine oxidation reaction(Hz OR) plays a crucial role in direct hydrazine fuel cells and holds promise for replacing the kinetics-sluggish oxygen evolution reaction in splitting water. While Ni–Zn alloys exhibit exceptional activity for Hz OR, their synthesis under mild conditions remains a challenge. Herein, a Ni–Zn nanosheet catalyst with Ni Zn inclusion was prepared on Ni foam by controllable chemical etching together with ethylene glycol reduction. X-ray diffraction and transmission electron microscopy confirmed the single-crystalline nature and the presence of intermetallic Ni Zn. The strong interaction between Ni and Zn O, along with defects, facilitated the formation of this intermetallic compound. The Ni–Zn/Ni foam exhibits remarkable catalytic activity(214.3m A cm-2at 0.1 V) and durability(87.8 % retention after 24 h) towards hydrazine electrooxidation, thanks to the combined benefits of intermetallic Ni Zn, mesoporous nanosheets, microscopic defects, single-crystalline characteristics, and a coherent Ni–Ni Zn interface. This study provides a new method for designing highly active Ni–Zn electrocatalysts for Hz OR.

关键词： Hydrazine electrooxidation Intermetallic NiZn single-crystalline Coherent interface Microscopic defects

Direct conversion of CO2 to CH4 on Pd/graphdiyne single-crystalline

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National Science Review 2024年第8期11卷 283-291页

作者： Chao Zhang Xuchen Zheng Yang Gao Chengyu Xing Siao Chen Yurui Xue Yuliang Li CAS Key Laboratory of Organic Solids Institute of ChemistryChinese Academy of Sciences Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringShandong University School of Chemical Sciences University of Chinese Academy of Sciences

A major impediment to the development of the efficient use of artificial photosynthesis is the lack of highly selective and efficient photocatalysts toward the conversion of CO2by sunlight energy at room temperature and ambient *** many years of hard work,we finally completed the synthesis of graphdiyne-based palladium quantum dot catalysts containing high-density metal atom steps for sele ctive artificial *** well-designed interface structure of the catalyst is composed of electron-donor and acceptor groups,resulting in the obvious incomplete charge-transfer phenomenon between graphdiyne and plasmonic metal nanostructures on the *** intrinsic characteristics are the origin of the high performance of the *** on its mechanism reveal that the synergism between 'hot electron' from local surface plasmon resonance and rapid photogenerated carrier separation at the ohmic contact interface accelerates the multi-electron reaction *** catalyst can selectively synthesize CH4directly from CO2and H2O with selectivity of near 100% at room temperature and pressure,and exhibits transformative performance,with an average CH4yield of 26.2 μmol g-1h-1and remarkable long-term stability.

关键词： graphdiyne controllable growth CO2 conversion single-crystalline heterocatalysis

Size controllable single-crystalline Ni-rich cathodes for high-energy lithium-ion batteries

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National Science Review 2023年第2期10卷 232-241页

作者： Ji-Lei Shi Hang Sheng Xin-Hai Meng Xu-Dong Zhang Dan Lei Xiaorui Sun Hongyi Pan Junyang Wang Xiqian Yu Chunsheng Wang Yangxing Li Yu-Guo Guo CAS Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry Chinese Academy of Sciences (CAS) University of Chinese Academy of Sciences Beijing Advanced Innovation Center for Materials Genome Engineering Institute of PhysicsCAS Department of Chemical and Biomolecular Engineering University of Maryland Chery New Energy Automobile Co. Ltd

A single-crystalline Ni-rich(SCNR) cathode with a large particle size can achieve higher energy density,and is safer,than polycrystalline ***,synthesizing large SCNR cathodes(>5 μm)without compromising electrochemical performance is very challenging due to the incompatibility between Ni-rich cathodes and high temperature ***,we introduce Vegard’s Slope as a guide for rationally selecting sintering aids,and we successfully synthesize size-controlled SCNR cathodes,the largest of which can be up to 10 μ*** theoretical calculation and experimental characterization show that sintering aids continuously migrate to the particle surface,suppress sublattice oxygen release and reduce the surface energy of the typically exposed facets,which promotes grain boundary migration and elevates calcination critical *** dense SCNR cathodes,fabricated by packing of different-sized SCNR cathode particles,achieve a highest electrode press density of 3.9 g cm-3and a highest volumetric energy density of 3000 Wh *** pouch cell demonstrates a high energy density of 303 Wh kg-1,730 Wh L-1and 76% capacity retention after 1200 *** cathodes with an optimized particle size distribution can meet the requirements for both electric vehicles and portable ***,the principle for controlling the growth of SCNR particles can be widely applied when synthesizing other materials for Li-ion,Na-ion and K-ion batteries.

关键词： lithium-ion baTheries high energy density Ni-rich cathodes single-crystalline surface energy

Unravelling a solution-based formation of single- crystalline kinked wurtzite nanowires： The case of MnSe

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Nano Research 2017年第7期10卷 2311-2320页

作者： Xinyi Yang Bo Zhou Chuang Liu Yongming Sui Guanjun Xiao Yingjin wei Xin Wang Bo Zou State Key Laboratory of Superhard Materials Jilin University Changchun 130012 China Laboratory of Physics and Technology for Advanced Barteries (Ministry of Education) Jilin University Changchun 130012 China College of Physics Jilin University Changchun 130012 China

The search for a novel strategy to sculpt semiconductor nanowires （NWs） at the atomistic scale is crucial for the development of new paradigms in optics, electronics, and spintronics. Thus far, the fabrication of single-crystalline kinked semiconductor NWs has been achieved mainly through the vapor-liquid-solid growth technique. In this study, we developed a new strategy for sculpting single-crystalline kinked wurtzite （WZ） MnSe NWs by triggering the nonpolar axial-oriented growth, thereby switching--at the atomistic scale---the NW growth orientation along the nonpolar axes in a facile solution-based procedure. This presents substantial challenges owing to the dominant polar c axis growth in the solution-based synthesis of one-dimensional WZ nanocrystals. More significantly, the ability to continuously switch the nonpolar axial-growth orientation allowed us to craft the kinking landscape of types 150°, 120°, 90°, and 60°. A probabilistic analysis of kinked MnSe NWs reveals the correlations of the synergy and interplay between these two sets of nonpolar axial growth-orientation switching, which determine the actual kinked motifs. Furthermore, discriminating the side-facet structures of the kinked NWs significantly strengthened the spatially selected interaction of Au nanoparticles. We envisage that such a facile solution-based strategy can be useful for synthesizing other single-crystalline kinked WZ-type transition-metal dichalcogenide NWs to develop novel functional materials with finely tuned properties.

关键词： kinked nanowires single-crystalline nonpolar axial growth wurtzite MnSe

Low-temperature growth of large-scale,single-crystalline graphene on Ir(111)

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Chinese Physics B 2019年第5期28卷 11-15页

作者： Hui Guo Hui Chen Yande Que Qi Zheng Yu-Yang Zhang Li-Hong Bao Li Huang Ye-Liang Wang Shi-Xuan Du Hong-Jun Gao Institute of Physics and University of Chinese Academy of Sciences CAS Center for Excellence in Topological Quantum Computation University of Chinese Academy of Sciences

Iridium is a promising substrate for self-limiting growth of graphene. However, single-crystalline graphene can only be fabricated over 1120 K. The weak interaction between graphene and Ir makes it challenging to grow graphene with a single orientation at a relatively low temperature. Here, we report the growth of large-scale, single-crystalline graphene on Ir(111) substrate at a temperature as low as 800 K using an oxygen-etching assisted epitaxial growth method. We firstly grow polycrystalline graphene on Ir. The subsequent exposure of oxygen leads to etching of the misaligned *** growth cycle, in which the leftover aligned domain serves as a nucleation center, results in a large-scale and single-crystalline graphene layer on Ir(111). Low-energy electron diffraction, scanning tunneling microscopy, and Raman spectroscopy experiments confirm the successful growth of large-scale and single-crystalline graphene. In addition, the fabricated single-crystalline graphene is transferred onto a SiO_2/Si substrate. Transport measurements on the transferred graphene show a carrier mobility of about 3300 cm^2·V^(-1)·s^(-1). This work provides a way for the synthesis of large-scale,high-quality graphene on weak-coupled metal substrates.

关键词： graphene low-temperature growth single-crystalline Ir(111)

Two highly porous single-crystalline zirconium-based metal-organic frameworks

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Science China Chemistry 2016年第8期59卷 980-983页

作者： Wen-Yang Gao Timmy Thiounn Lukasz Wojtas Yu-Sheng Chen Shengqian Ma Department of Chemistry University of South Florida Florida 33620 USA ChemMatCARS Center for Advanced Radiation Sources University of Chicago Illinois 60439 USA

Herein we report two highly porous Zr-based metal-organic frameworks （MOFs, 1 and 2） constructed by the truncated octahedral secondary building unit （SBU） of Zr604（OH）4（CO2）12 and the organic linear ligand of 4,4＇-stilbenedicarboxylic acid （H2sbdc） or 4,4＇-azobenezenedicarboxylic acid （H2abdc）. Both Zr-based MOFs are obtained as single crystals of suitable size for single-crystal X-ray diffraction analysis. Furthermore, these two Zr-based MOFs have been fully characterized by powder X-ray diffraction （PXRD） studies, thermogravimetric analysis （TGA）, infrared spectroscopy （IR） and gas adsorption analysis. In particular, their CO2 gas adsorption behaviors have been investigated and discussed.

关键词： metal-organic frameworks zirconium cluster single-crystalline

Crack-free single-crystalline Co-free Ni-rich LiNi_(0.95)Mn_(0.05)O_(2) layered cathode

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eScience 2022年第1期2卷 116-124页

作者： Lianshan Ni Ruiting Guo Susu Fang Jun Chen Jinqiang Gao Yu Mei Shu Zhang Wentao Deng Guoqiang Zou Hongshuai Hou Xiaobo Ji State Key Laboratory of Powder Metallurgy College of Chemistry and Chemical EngineeringCentral South UniversityChangshaHunan410083PR China

The rapid growth in global electric vehicles(EVs)sales has promoted the development of Co-free,Ni-rich layered cathodes for state-of-the-art high energy-density,inexpensive lithium-ion batteries(LIBs).However,progress in their commercial use has been seriously hampered by exasperating performance deterioration and safety ***,a robust single-crystalline,Co-free,Ni-rich LiNi_(0.95)Mn_(0.05)O_(2)(SC-NM95)cathode is successfully designed using a molten salt-assisted method,and it exhibits better structural stability and cycling durability than those of polycrystalline LiNi_(0.95)Mn_(0.05)O_(2) (PC-NM95).Notably,the SC-NM95 cathode achieves a high discharge capacity of 218.2 mAh g^(-1),together with a high energy density of 837.3 Wh kg^(-1) at 0.1 C,mainly due to abundant Ni^(2+)/Ni^(3+) *** also presents an outstanding capacity retention(84.4%)after 200 cycles at 1 C,because its integrated single-crystalline structure effectively inhibits particle microcracking and surface phase *** contrast,the PC-NM95 cathode suffers from rapid capacity fading owing to the nucleation and propagation of intergranular microcracking during cycling,facilitating aggravated parasitic reactions and rocksalt phase *** work provides a fundamental strategy for designing high-performance singlecrystalline,Co-free,Ni-rich cathode materials and also represents an important breakthrough in developing high-safe,low-cost,and high-energy LIBs.

关键词： single-crystalline Co-free Ni-rich cathodes Intergranular microcracking H2↔H3 phase transition Cycling stability

Sodium ion storage performance and mechanism in orthorhombic V_(2)O_(5) single-crystalline nanowires

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Science China Materials 2021年第3期64卷 557-570页

作者： Yanwei Li Jingcheng Ji Jinhuan Yao Ying Zhang Bin Huang Guozhong Cao Guangxi Key Laboratory of Electrochemical and Magneto-chemical Functional Materials College of Chemistry and BioengineeringGuilin University of TechnologyGuilin541004China Department of Materials Science and Engineering University of WashingtonSeattleWA98195USA

A fundamental understanding of the electrochemical reaction process and mechanism of electrodes is very crucial for developing high-performance electrode *** this study,we report the sodium ion storage behavior and mechanism of orthorhombic V_(2)O_(5) single-crystalline nanowires in the voltage window of 1.0–4.0 V(***/Na+).The single-crystalline nanowires exhibit a large irreversible capacity loss during the first discharge/charge cycle,and then show excellent cycling stability in the following *** a current density of 100 mA g^(−1),the nanowires electrode delivers initial discharge/charge capacity of 217/88 mA h g^(−1),corresponding to a Coulombic efficiency of only 40.5%;after 100 cycles,the electrode remains a reversible discharge capacity of 78 mA h g^(−1) with a fading rate of only 0.09%per cycle compared with the 2nd cycle discharge *** sodium ion storage mechanism was investigated,illustrating that the large irreversible capacity loss in the first cycle can be attributed to the initially formed single-crystalline α′-Nax V_(2)O_(5)(0.02single-phase(solid solution)reaction,leading to excellent cycling *** Na^(+) diffusion coefficient in α′-Nax V_(2)O_(5) ranges from 10^(−12) to 10^(−11.5) cm^(2) s^(−1) as evaluated by galvanostatic intermittent titration technique(GITT).

关键词： sodium ion batteries V_(2)O_(5) single-crystalline nanowires sodium storage mechanism