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Improvement of the Selectivity for Hydrogen Peroxide Production via the Synergy of TiO2 and Graphene

Chinese Journal of Structural Chemistry 2022年第3期41卷 85-91,I0009页

作者： SUN Yun-Long HUANG Jun-Heng CAS Key Laboratory of Design and Assembly of Functional Nano-structures Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fuzhou University Fuzhou 350108China

To replace the four-electron transferred pathway of oxygen reduction reaction(ORR)by two-electron transferred pathway of ORR(2e-ORR)is desirable for the production of hydrogen peroxide with *** development of electrocatalysts with high selectivity toward 2e-ORR is of great interest but it is still a ***,we synthesized the graphene-supported titanium dioxide nanocomposite as the 2e-ORR catalysts by a combinative process of hydrothermal methods and *** to the synergistic effect between the graphene with high conductivity and the titanium dioxide with defect sites,the composite TiO_(2)/graphene exhibits the improved selectivity(up to 90%)for oxygen converting into hydrogen peroxide.

关键词： oxygen reduction reaction hydrogen peroxide titanium dioxide graphene electrochemistry

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Fluorinated N,P co-doped biomass carbon with high-rate performance as cathode material for lithium/fluorinated carbon battery

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Rare Metals 2025年第1期44卷 110-120页

作者： Ke Yan Yan Zou Liang-Xue Bao Qi Xia Ling-Yi Meng Hai-Chen Lin Hui-Xin Chen Hong-Jun Yue College of Chemistry Fuzhou UniversityFuzhou 350108China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research On the Structure of MatterChinese Academy of SciencesFuzhou 350002China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamen 361021China Sustainable Power and Energy Center Nano Engineering DepartmentUniversity of California San DiegoLa JollaSan DiegoCA 92093USA

Lithium/fluorinated carbon(Li/CF_(x))batteries are greatly limited in their applications mostly due to poor rate *** this study,N,P co-doped biomass carbon was synthesized using melamine and phytic acid as doping sources,and the resulting product was then utilized as a precursor for CF_(x).The resulting fluorinated biomass carbon has a high degree of fluorination,exceeding the specific capacity of commercial fluorinated graphite while also demonstrating exceptional performance at high discharge *** the fluorination process,N,P-containing functional groups were removed from the crystalline lattice in the basal *** facilitates the formation of a defect-rich carbon matrix,enhancing the F/C ratio by improving the fluorinated active sites and obtaining more highly active semi-ionic ***,the abundant defects and porous structure promote Li^(+)*** functional theory calculations indicated that doping modification effectively reduces the energy barrier for Li+migration,enhancing Li+transport *** prepared CF_(x)delivers material with a maximum specific capacity of 919 mAh·g^(-1),while maintaining a specific capacity of 702 mAh·g^(-1)at a high discharge current density of 20C(with a capacity retention rate of 76.4%).In this study,fluorinated N,P co-doped biomass carbon,exhibiting ultrahigh capacity and high-rate performance,was prepared for the first time,which can potentially advance the commercialization of CF_(x).

关键词： Li/CF_(x)primary batteries Biomass carbon Heteroatom doping High performance

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Si Doping-Induced Electronic Structure Regulation of Single-Atom Fe Sites for Boosted CO_(2) Electroreduction at Low Overpotentials

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Research 2023年第4期2023卷 307-319页

作者： Changsheng Cao Shenghua Zhou Shouwei Zuo Huabin Zhang Bo Chen Junheng Huang Xin-Tao Wu Qiang Xu Qi-Long Zhu State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China University of Chinese Academy of Science Beijing100049China KAUST Catalysis Center(KCC) King Abdullah University of Science and Technology(KAUST)Thuwal23955-6900Saudi Arabia Department of Chemistry City University of Hong KongHong Kong999077China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of NanomaterialsFujianInstitute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou350108China Institute for Integrated CellMaterial Sciences(iCeMS) Kyoto UniversityKyoto 606-8501Japan Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials(SKLPM) SUSTech-Kyoto University Advanced Energy Materials Joint Innovation Laboratory(SKAEM-JIL)and Department of Materials Science and EngineeringSouthern University of Science and Technology(SUSTech)Shenzhen518055China

Transition metal-based single-atom catalysts(TM-SACs)are promising alternatives to Au-and Ag-based electrocatalysts for CO production through CO_(2)reduction ***,developing TM-SACs with high activity and selectivity at low overpotentials is ***,a novel Fe-based SAC with Si doping(Fe-N-C-Si)was prepared,which shows a record-high electrocatalytic performance toward the CO_(2)-to-CO conversion with exceptional current density(>350.0 mA cm^(−2))and~100%Faradaic efficiency(FE)at the overpotential of<400 mV,far superior to the reported Fe-based *** assembling Fe-N-C-Si as the cathode in a rechargeable Zn-CO_(2)battery delivers an outstanding performance with a maximal power density of 2.44 mW cm^(−2)at an output voltage of 0.30 V,as well as high cycling stability and FE(>90%)for CO *** combined with theoretical analysis unraveled that the nearby Si dopants in the form of Si-C/N bonds modulate the electronic structure of the atomic Fe sites in Fe-N-C-Si to markedly accelerate the key pathway involving^(*)CO intermediate desorption,inhibiting the poisoning of the Fe sites under high CO coverage and thus boosting the CO_(2)RR *** work provides an efficient strategy to tune the adsorption/desorption behaviors of intermediates on singleatom sites to improve their electrocatalytic performance.

关键词： desorption bonds exceptional

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Hybrid of Quaternary Layered Double Hydroxides and Carbon nanotubes for Oxygen Evolution Reaction

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Chinese Journal of Structural Chemistry 2020年第10期39卷 1807-1816,1742页

作者： FU Chang-Le WANG Yi HUANG Jun-Heng Fujian Normal University Fuzhou 350007China CAS Key Laboratory of Design and Assembly of Functional Nano-structures Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Highly active electrocatalysts based on Layered Double Hydroxides(LDH)towards oxygen evolution reactions(OER)are required for the applications of renewable energy-conversion *** improvement of conductivity and electron-transporting capability for LDH materials remains an enormous challenge ***,we synthesized carbon nanotube supported quaternary FeCoNiW-LDH ultrathin nanosheets with 1 nm thickness via one-pot hydrothermal methods,which exhibit enhanced OER activity due to the synergistic effect of modified CNTs and doped W^6+onto LDH nanosheets *** loaded carbon nanotubes can directly result in the improved *** addition,W^6+doping in LDH can modify the electronic structure and further enhance the conductivity of ***-LDH/CNT exhibits a small overpotential(258 mV)at a current density of 10 mA·cm^–2 and low Tafel slope(41 mV decade^–1)towards OER in alkaline solutions,outperforming the noble metal RuO2 catalysts.

关键词： FeCoNiW layered double hydroxide electrocatalyst reduced carbon nanotube tungsten doping oxygen evolution reaction

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Dispersion-Selective Band Engineering in an Artificial Kagome Superlattice

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Physical Review Letters 2024年第6期133卷 066302-066302页

作者： Shuai Wang Zhen Zhan Xiaodong Fan Yonggang Li Pierre A. Pantaleón Chaochao Ye Zhiping He Laiming Wei Lin Li Francisco Guinea Shengjun Yuan Changgan Zeng CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics and Department of Physics International Center for Quantum Design of Functional Materials (ICQD) Hefei National Research Center for Physical Sciences at the Microscale Key Laboratory of Artificial Micro- and Nano-structures of the Ministry of Education and School of Physics and Technology Madrid 28015 Spain School of Advanced Manufacturing Engineering Hefei National Laboratory Paseo Manuel de Lardizabal 4 San Sebastian 20018 Spain Wuhan Institute of Quantum Technology Wuhan Hubei 430206 China

The relentless pursuit of band structure engineering continues to be a fundamental aspect in solid-state research. Here, we meticulously construct an artificial kagome potential to generate and control multiple Dirac bands of graphene. This unique high-order potential harbors natural multiperiodic components, enabling the reconstruction of band structures through different potential contributions. As a result, the band components, each characterized by distinct dispersions, shift in energy at different velocities in response to the variation of artificial potential. Thereby, we observe a significant spectral weight redistribution of the multiple Dirac peaks. Furthermore, the magnetic field can effectively weaken the superlattice effect and reactivate the intrinsic Dirac band. Overall, we achieve actively dispersion-selective band engineering, a functionality that would substantially increase the freedom in band design.

关键词： Electronic structure Flat bands Local density of states Transport phenomena 2-dimensional systems Graphene Kagome lattice Band structure methods Tight-binding model Transport techniques

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D^(6h)Symmetric Radical Donor-Acceptor nanographene Modulated Interfacial Carrier Transfer for High-Performance Perovskite Solar Cells

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CCS Chemistry 2023年第9期5卷 2159-2170页

作者： Can Wang Yifeng Gao Zhen-Lin Qiu Ping-Ping Sun Naoyuki Shibayama Zilong Zhang Qiu Xiong Fangbin Ren Shui-Yang Lien Lusheng Liang Jiaoxia Zhang Yuan-Zhi Tan Peng Gao CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 Laboratory for Advanced Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021 University of Chinese Academy of Sciences Beijing 100049 School of Materials Science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003 Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory for Physical Chemistry of Solid SurfacesEngineering Research Center for Nano-Preparation Technology of Fujian ProvinceDepartment of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005 Department of Chemistry School of ScienceHainan UniversityHaikou 570228 Faculty of Biomedical Engineering Graduate School of EngineeringToin University of YokohamaYokohamaKanagawa 225-8503 Xiamen University of Technology Xiamen 361024

Imbalanced charge-carrier extraction remains an issue aggravating interfacial charge accumulation and *** hopping transport channels could accelerate the extraction of ***,we demonstrated an effective“bridging interface”strategy between the perovskite/2,2′,7,7′-tetrakis(N,N-di-pmethoxyphenylamine)-9,9′-spirobifluorene(spiro-OMeTAD)that modulates interfacial charge transfer and improves hole mobility using radical-containing donor-acceptor nanographenes(D-A NGs)possessing electron-deficient perchlorinated NGs and electron-rich aniline *** fully delocalized backbone of nanographene formed a conjugated bridge for intermolecular charge transfer and generated stable radical cations,verified by electron spin *** andπ-πstacking orientation of D-A NGs also provided advantageous hopping transport *** favorable charge transfer within D-A NGs,systematic explorations indicated a strong interface coupling and noticeable charge transfer across the D-A NGs and perovskite interface,where electrons would flow from D-A NGs to perovskite,and holes would flow from perovskite to D-A ***,the hole mobility of spiro-OMeTAD was also enhanced because the D-A NGs would diffuse into the spiro-OMeTAD *** a result,planar n-i-p perovskite solar cellsmodified byD-ANG-OMe/D-ANG-tBudeliveredchampion power conversion efficiencies(PCEs)of 23.25%and 23.51%,respectively.

关键词： perovskite solar cell radicals donor-acceptor nanographene hole mobility interfacial charge transfer

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Coexistence of Robust Edge States and Superconductivity in Few-Layer Stanene

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Physical Review Letters 2022年第20期128卷 206802-206802页

作者： Chenxiao Zhao Leiqiang Li Liying Zhang Jin Qin Hongyuan Chen Bing Xia Bo Yang Hao Zheng Shiyong Wang Canhua Liu Yaoyi Li Dandan Guan Ping Cui Zhenyu Zhang Jinfeng Jia Key Laboratory of Artificial Structures and Quantum Control (Ministry of Education) Shenyang National Laboratory for Materials Science School of Physics and Astronomy Shanghai Jiao Tong University Shanghai 200240 China International Center for Quantum Design of Functional Materials (ICQD) Hefei National Laboratory for Physical Sciences at Microscale (HFNL) and CAS Center for Excellence in Quantum Information and Quantum Physics University of Science and Technology of China Hefei Anhui 230026 China Key Laboratory for Special Functional Materials of Ministry of Education Collaborative Innovation Center of Nano Functional Materials and Applications School of Materials Science and Engineering Henan University Kaifeng 475004 China International Laboratory for Quantum Functional Materials of Henan and School of Physics and Microelectronics Zhengzhou University Zhengzhou 450001 China Tsung-Dao Lee Institute Shanghai Jiao Tong University Shanghai 200240 China CAS Center for Excellence in Topological Quantum Computation University of Chinese Academy of Sciences Beijing 100190 China

High-quality stanene films have been actively pursued for realizing not only quantum spin Hall edge states without backscattering, but also intrinsic superconductivity, two central ingredients that may further endow the systems to host topological superconductivity. Yet to date, convincing evidence of topological edge states in stanene remains to be seen, let alone the coexistence of these two ingredients, owing to the bottleneck of growing high-quality stanene films. Here we fabricate one- to five-layer stanene films on the Bi(111) substrate and observe the robust edge states using scanning tunneling microscopy/spectroscopy. We also measure distinct superconducting gaps on different-layered stanene films. Our first-principles calculations further show that hydrogen passivation plays a decisive role as a surfactant in improving the quality of the stanene films, while the Bi substrate endows the films with nontrivial topology. The coexistence of nontrivial topology and intrinsic superconductivity renders the system a promising candidate to become the simplest topological superconductor based on a single-element system.

关键词： Growth Topological insulators Elemental superconductors Stanene Topological superconductors First-principles calculations Molecular beam epitaxy Scanning tunneling microscopy Scanning tunneling spectroscopy

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designing of covalent organic framework/2D g-C 3 N 4 heterostructure using a simple method for enhanced photocatalytic hydrogen production

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Journal of Colloid and Interface Science 2024年 653卷 1650-1661页

作者： Ahmed E. Hassan Ahmed M. Elewa Mai S.A. Hussien Ahmed F.M. EL-Mahdy Islam M.A. Mekhemer Ibrahim S. Yahia Tarek A. Mohamed Ho-Hsiu Chou Zhenhai Wen CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China University of Chinese Academy of Sciences Beijing 100049 China Department of Chemistry Faculty of Science Al-Azhar University Nasr City 11884 Cairo Egypt Department of Chemical Engineering National Tsing Hua University Hsinchu 300044 Taiwan Nuclear Chemistry Department Hot Laboratories Center Atomic Energy Authority Cairo 13759 Egypt Nanoscience Laboratory for Environmental and Biomedical Applications (NLEBA) Semiconductor Lab Department of Physics Faculty of Education Ain Shams University Roxy Cairo 11757 Egypt Department of Chemistry Faculty of Education Ain Shams University Roxy Cairo 11757 Egypt Department of Materials and Optoelectronic Science National Sun Yat-Sen University Kaohsiung 80424 Taiwan Laboratory of Nano-Smart Materials for Science and Technology (LNSMST) Department of Physics Faculty of Science King Khalid University P.O. Box 9004 Abha Saudi Arabia Research Center for Advanced Materials Science (RCAMS) King Khalid University Abha 61413 P.O. Box 9004 Saudi Arabia Center of Medical and Bio-Allied Health Sciences Research (CMBHSR) Ajman University Ajman P.O. Box 346 United Arab Emirates

designing heterostructure photocatalysts is a promising approach for developing highly efficient photocatalysts for hydrogen energy production. In this work, we synthesized a series of a covalent organic framework (COF)/g-C 3 N 4 (CN) heterojunction photocatalysts, denoted as x % COF/CN (in which x indicates the weight % of COF and x = 5, 10, 20, 30, 40, 50, 90, 95, 100), for hydrogen production . The COF, which is a key component of the photocatalyst, was prepared by assembling benzothiadiazole (BT) and pyrene (Py) derivatives as building blocks. Integrating COF rods into the two-dimensional (2D) layered g-C 3 N 4 structure significantly improved photocatalytic H 2 production. The hybrid system (30 % COF/CN) displayed an outstanding hydrogen evolution rate (HER) of 27540 ± 805 μmol g −1 h −1 , outperforming most known COFs and g-C 3 N 4 -based photocatalysts, besides exhibiting stable photocatalytic performance. Moreover, the apparent quantum yield (AQY) was 15.5 ± 0.8 % at 420 nm. Experimental techniques and density functional theory (DFT) calculations demonstrated that the 30 % COF/CN heterostructure has broad visible-light absorption, adequate band energy levels, and the best chemical reactivity descriptors compared to the individual components, resulting in effective carrier separation and excellent performance. Our findings offer a valuable strategy for developing highly efficient and stable heterojunction photocatalysts for visible-light‐driven H 2 evolution.

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Controlling disorder in host lattice by hetero-valence ion doping to manipulate luminescence in spinel solid solution phosphors

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Science China Chemistry 2018年第12期61卷 1624-1629页

作者： Qinqin Ma Jie Wang Wei Zheng Qian Wang Zhiheng Li Hengjiang Cong Huijun Liu Xueyuan Chen Quan Yuan Key Laboratory of Analytical Chemistry for Biology and Medicine(Ministry of Education) College of Chemistry and Molecular SciencesWuhan University CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Key Laboratory of Artificial Micro-and Nano-Structures of Ministry of Education and School of Physics and Technology Wuhan University

Phosphor materials have been rapidly developed in the past decades. Developing phosphors with desired properties including strong luminescence intensity and long lifetime has attracted widespread attention. Herein, we show that hetero-valence ion doping can serve as a potent strategy to manipulate luminescence in persistent phosphors by controlling disorder in the host lattice. Specifically, spinel phosphor Zn(Ga_(1-x)Zn_x)(Ga_(1-x)Ge_x)O_4:Cr is developed by doping ZnGa_2O_4:Cr with tetravalent Ge^(^(4+)).Compared to the original ZnGa_2O_4:Cr, the doped Zn(Ga_(1-x)Zn_x)(Ga_(1-x)Ge_x)O_4:Cr possesses significantly enhanced persistent luminescence intensity and prolonged decay time. Rietveld refinements show that Ge^(4+)enters into octahedral sites to substitute Ga^(3+), which leads to the co-substitution of Ga^(3+) by Zn^(2+) for charge compensation. The hetero-valence substitution of Ga^(3+) by Ge^(4+)and Zn^(2+) enriches the charged defects in Zn(Ga_(1-x)Zn_x)(Ga_(1-x)Ge_x)O_4:Cr, making it possible to trap large amounts of charge carriers within the defects during excitation. Electron paramagnetic resonance measurement further confirms that the amount of Cr^(3+) neighboring charged defects increases with Ge^(4+)doping. Thus charge carriers released from defects can readily combine with the neighboring Cr^(3+) to produce bright persistent luminescence after excitation ceases. The hetero-valence ion doping strategy can further be employed to develop many other phosphors and contributes to lighting, photocatalysis and bioimaging.

关键词： persistent luminescence nanoparticle defect doping

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Investigation of sustainable rare earth recovery on carbon electrodes by electrosorption and precipitation coupling strategy

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Journal of Environmental Chemical Engineering 2025年第4期13卷

作者： Yanxin Wang Peilin Lei Yujun Chai Xiaoqi Sun College of Chemistry and Materials Science Hebei Normal University Shijiazhuang Hebei 050024 PR China Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen 361021 PR China Hebei Key Laboratory of Inorganic Nano-materials Hebei Normal University Shijiazhuang Hebei 050024 PR China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 PR China University of Chinese Academy of Sciences Beijing 100049 PR China

This study investigates the recovery of rare earth (RE) using a coupling electrosorption and precipitation strategy. The electrochemical behavior and recovery properties of various materials, i.e., activated carbon, carbon nanofibers, carbon nanotubes, graphene, and porous carbon, were evaluated. They show the good crystalline, amorphous or the coexistence of two states. The reaction occurred on grapheme and carbon nanofiber within the scan range, but it shows the capacitive behavior for other three. The electrosorption-precipitation coupling capacity and removal efficiency varied due to the cooperation of applied voltage and inner voltage, in addition to the effect of functional groups, defects and conductivity. During the process, rare earth ions were first adsorbed onto the electrode surface and then reacted with OH - ions to form precipitates. Meanwhile, oxygen was generated at the Pt electrode, while only trace amounts of hydrogen were observed on the working electrode due to the involvement of NO 3 - ions. Additionally, La(Ⅲ), Ce(Ⅲ), Pr(Ⅲ) and Nd(Ⅲ) ions were effectively recovered and enriched using carbon-based electrodes, with capacities of 2064.5, 2305.8, 2198.7, and 2288.9 mg·g −1 , respectively, in a 0.01 mol·L −1 RE solution. These findings suggest that the selection of materials with larger specific surface areas, high electrical conductivity, more defects, effective functional groups and low potential can reduce internal voltage, enhance reaction driving forces, and improve recovery efficiency. The recovery process has sustainable RE separation characteristics, with no volatile organic solvent (VOC), acid and alkali consumption, or wastewater.

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