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Enhanced CO2 Electrolysis with Metal-oxide Interface Structures

Chinese Journal of Structural Chemistry 2021年第1期40卷 31-41,1页

作者： XU Ze-Tong XIE Kui College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China 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

The ever-decreasing fossil fuels and the increasing greenhouse effect have caused substantial *** oxide electrolyser cell(SOEC)with La_(0.75)Sr_(0.25)Cr_(0.5 )Mn_(0.5)O_(3-δ)(LSCM)as a cathode was used for CO_(2) electrolysis to *** this work,the metal-oxide interface was constructed on the LSCM framework by in-situ exsolution and impregnation,and the uniform distribution of metal nanoparticles on the LSCM framework was confirmed by spectroscopy techniques and electron microscopy *** existence of three-phase boundary promoted the absorption and electrolysis of CO_(2).(La_(0.75) Sr_(0.25))0.9(Cr_(0.5 )Mn_(0.5))_(0.9)(Ni_(0.5) Cu_(0.5))_(0.1) O_(3-δ)(LSCMNC)showed the best electrolytic CO_(2) performance at 850℃and exhibited excellent electrocatalytic activity after 100 hours of long-term testing and 8 redox cycles.

关键词： solid oxide electrolyser cell LSCM metal nanoparticles CO_(2)electrolysis

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Copper fluoride as a low-cost sodium-ion battery cathode with high capacity

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Chinese Chemical Letters 2022年第3期33卷 1435-1438页

作者： Yiming Dai Qiujie Chen Chenchen Hu Yangyang Huang Wangyan Wu Mingliang Yu Dan Sun Wei Luo Institute of New Energy for Vehicles School of Materials Science and EngineeringTongji UniversityShanghai 201804China 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 Haixi Institute Xiamen Institute of Rare Earth MaterialsChinese Academy of SciencesXiamen 361021China

Sodium-ion batteries (SIBs) are promising alternatives to lithium-ion batteries (LIBs) for large-scale energy storage considering the abundance and low cost of Na-containing resources. However, the energy density of SIBs has been limited by the typically low specific capacities of traditional intercalation-based cathodes. Metal fluorides, in contrast, can deliver much higher capacities based on multi-electron conversion reactions. Among metal fluorides, CuF_(2) presents a theoretical specific capacity as high as 528 mAh/g while its Na-ion storage mechanism has been rarely reported. Here, we report CuF_(2) as a SIB cathode, which delivers a high capacity of 502 mAh/g but suffers from poor electrochemical reversibility. As a solution, we adjust the cell configuration by inserting a carbon-coated separator, which hinders the transportation of dissolved Cu ions and improves the reversibility of the CuF_(2) cathode. By using in-situ XRD measurements and theoretical calculation, we propose that a one-step conversion reaction occurs during the discharge process, and a reconversion reaction competes with the oxidization of Cu to dissolved Cu ion during the charge process.

关键词： Sodium-ion battery Copper fluoride Cathode Energy density Conversion reaction

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Luminescent nano-bioprobes based on NIR dye/lanthanide nanoparticle composites

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Aggregate 2021年第5期2卷 115-131页

作者： Shan Lu Jianxi Ke Xingjun Li Datao Tu Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFujianChina Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China FujianChina

Near-infrared(NIR)light,which has ignorable tissue scattering/absorption,minimal photodamage,and no autofluorescence interference,is highly favorable for *** dye and lanthanide-doped nanoparticle(LnNP),as representative NIR-excited luminescence probes,have attracted increasing interest due to their unique optical property and low biological *** of luminescence probes based on NIR dye/LnNP nanocomposites cannot only integrate the advantages but also achieve additional functions via regulating internal energy transfer *** this review,we focus on the most recent advances in the development of NIR dye/LnNP nanocomposites as potential bioprobes,which cover from their fundamental photophysics to bioapplications,including energy transfer mechanisms,interface engineering(involving binding interaction,distance,and aggregation as key factors),and their applications for dye-sensitized upconversion/downshifting luminescent bioimaging,detection of biomolecules,and NIR-triggered diagnosis and *** future prospects and efforts toward this active research field are also envisioned.

关键词： dye sensitization energy transfer interface engineering lanthanide-doped nanoparticle nano-bioprobe NIR dye

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Neodymium and samarium codoped PLZT ferroelectric ceramics for potential betavoltaic nuclear batteries

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Journal of Rare Earths 2023年第10期41卷 1583-1589,I0004页

作者： Zhixiong Song Jizhen Liu Liyan Xue Zhengming Jiang Fan Yang Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou350108China 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 SciencesFuzhou350002China Fujian Province Joint Innovation Key Laboratory of Fuel and Materials in Clean Nuclear Energy System Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China Xiamen Institute of Rare Earth Materials Haixi InstituteChinese Academy of SciencesXiamen361021China Nuclear Power Institute of China Chengdu610000China Sichuan Jcc Rare Earth Metals New Material Co. Ltd.Chengdu610000China

In this work,neodymium(Nd)and samarium(Sm)codoped lead lanthanum zirconate titanate(PLZT)ceramics were prepared by a high-temperature solid-state *** samples were characterized by X-ray diffraction,scanning electron microscopy and ferroelectric *** earth-doped PLZT ceramics show good phase *** appropriate rare earth element doping amount increases the densities of PLZT ceramics and reduces their resistivities,which is due to the role of rare earth elements in grain ***,the increase in the amount of grain boundaries caused by grain refinement also affects domain ***,with increasing doping concentration,the remnant polarization of PLZT gradually decreases,and the doping of rare earth elements also slightly reduces the band gap of *** irradiation with an X-ray simulated beta source with a particle energy of 10 keV(between the average energies of the beta particles of^3H and^(63)Ni),the ceramic sheets in this work produce current densities of up to 1.38 nA/cm^*** indicates that Nd and Sm codoped PLZT ceramics have a certain potential for application in betavoltaic batteries.

关键词： Betavoltaic battery Rare earths Ferroelectric X-ray

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Electro-optic modulation of solution-processed molybdenum disulfide

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Physical Review Applied 2024年第3期22卷 034057页

作者： Songwei Liu Yingyi Wen Jingfang Pei Xiaoyue Fan Yongheng Zhou Yang Liu Ling-Kiu Ng Yue Lin Teng Ma Panpan Zhang Xiaolong Chen Gang Wang Guohua Hu Department of Electronic Engineering Centre for Quantum Physics Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurement (MOE) School of Physics Department of Electrical and Electronic Engineering Shun Hing Institute of Advanced Engineering CAS Key Laboratory of Design and Assembly of Functional Nanostructures and State Key Laboratory of Structural Chemistry Department of Applied Physics State Key Laboratory of Information Photonics and Optical Communications

Solution-processed molybdenum disulfide (MoS2) shows promise for tunable photonics and optoelectronics development. However, though scalable, it often leads to devices with inferior performance as a result of its random, discrete nature. In this study, we show via density-functional-theory calculations that the electronic structure of the individual solution-processed nanosheets can be modulated collectively by external electric fields. Particularly, the nanosheets can form Stark ladders, giving variations in the underlying optical processes and thus tunable collective optical properties. We confirm this electro-optical modulation experimentally using solution-processed MoS2 films with ferroelectric poly(vinylidene fluoride-co-trifluoroethylene) [P(VDF-TrFE)] incorporated, and prove that the local polarization fields from P(VDF-TrFE) can modulate the collective optical properties of the MoS2, specifically, the optical absorption and photoluminescence. Given the scalability of solution processing, our results underpin the potential of electro-optical modulation of solution-processed MoS2 for tunable photonics and optoelectronics development. To illustrate this potential, we demonstrate solution-processed electroabsorption modulators.

关键词： Electric field effects Electro-optic effects Optoelectronics Photonics 2-dimensional systems Layered semiconductors Transition metal dichalcogenides Chemical solution deposition

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Efficient oxygen reduction through metal-free 3D covalent organic frameworks:a novel approach

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Science China Materials 2024年第11期67卷 3589-3595页

作者： Shanyue Wei Xiaowei Wu Shufei Zhu Zhiyang Wang Jiangli Wang Can-Zhong Lu Yiming Xie Engineering Research Center of Environment-Friendly Function Materials Ministry of EducationCollege of Materials Science&EngineeringHuaqiao UniversityXiamen 361021China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of NanomaterialsState Key Laboratory of Structural ChemistryFujian 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 University of Chinese Academy of Sciences Beijing 100049China

Covalent organic framework(COF)materials have gained significant applications in electrocatalytic systems due to their structural diversity and tunable ***,three-dimensional(3D)COFs exhibit multistage pore structures,exposing numerous open sites,which facilitate the oxygen reduction reaction(ORR)***,the advancement of 3D COFs for ORR has been hindered by challenges,including limited topologies,the scarcity of building blocks with the required reactivity and symmetries,and difficulties in determining crystalline *** this work,we utilized an 8-connectivity building unit and successfully constructed two isoreticular 3D COF materials,which exhibited exceptionally high catalytic activity for 2e−oxygen reduction reaction without the addition of any metal or conductive support materials,nor the pyrolyzed *** electrochemically active surface areas(ECSAs)of the two 3D COFs were found to be 17.19 and 12.18 mF/cm2,respectively,which were significantly higher than those reported from other framework materials.

关键词： electrocatalysis oxygen reduction reaction metalfree covalent organic framework

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Precise Construction of Stable Bimetallic Metal–Organic Frameworks with Single-Site Ti(IV) Incorporation in Nodes for Efficient Photocatalytic Oxygen Evolution

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CCS Chemistry 2022年第8期4卷 2782-2792页

作者： Lan Li Zhi-Bin Fang Wenzhuo Deng Jun-Dong Yi Rui Wang Tian-Fu Liu State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002 University of Chinese Academy of Sciences Beijing 100049 CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002

Assembling the reactive low-cost Co clusters and photoresponsive ligands in the form of metal–organic frameworks(MOFs)is a promising strategy to construct efficient water-oxidizing photocatalysts,but it is restricted by poor water *** high valent cations in the clusters to build heterometallic Co-MOFs might be a solution,yet a precise fabrication strategy is still challenging.

关键词： cobalt catalyst metal–organic frameworks single-site Ti incorporation stability photocatalytic O_(2)evolution

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Lanthanide nanoparticles ignite dark molecular triplets

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Science China Chemistry 2021年第4期64卷 511-512页

作者： Jin Xu Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures State Key Laboratory of Structural Chemistryand Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Molecular triplets have attracted great interest across multidisciplinary fields of the research ranging from thermally activated delayed fluorescence[1],triplet-triplet annihilation(TTA)upconversion[2],to photodynamic therapy relying on TTA between triplet photosensitizers and surrounding triplet oxygen to generate singlet oxygen species[3].

关键词： triplet Lanthanide annihilation

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Boosting the Energy Migration Upconversion through Inter-Shell Energy Transfer in Tb^(3+)-Doped Sandwich Structured Nanocrystals

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CCS Chemistry 2022年第6期4卷 2031-2042页

作者： Dan Xu Jin Xu Xiaoying Shang Shaohua Yu Wei Zheng Datao Tu Renfu Li Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 University of Chinese Academy of Sciences Beijing 100049 Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China FuzhouFujian 350108

It remained challenging to fabricate Tb^(3+)-doped lanthanide nanocrystals(NCs)to simultaneously acquire strong energy migration upconversion(EMU)emissions of Tb^(3+)while suppressing the Tm3+UV upconversion emissions that cause background biofluorescence issues in bioapplications based on Tb^(3+)-doped EMU ***,we report a novel sandwich structured core@shell@shell scheme for the design of EMU NCs,for example,NaLuF4∶Yb/Gd@NaGdF4∶Tm@NaLuF4∶Tb NCs,wherein Yb^(3+),Tm^(3+),and Tb^(3+)are incorporated separately into the inner core,middle shell,and outer shell,*** found that in the sandwich structured NCs,the effective inter-shell energy transfer from Gd^(3+)in the middle shell to Tb^(3+)in the outer shell accelerated the Yb^(3+)-Tm^(3+)five-photon upconversion and the subsequent Tm^(3+)to Gd^(3+)energy transfer processes,which could eventually lead to almost complete inhibition of Tm^(3+)UV upconversion emissions,concurrent with the strong EMU emissions of Tb^(3+).Our findings might stimulate new concepts for manipulating upconversion emissions of lanthanide NCs.

关键词： lanthanide nanocrystals energy migration upconversion sandwich structured inter-shell energy transfer energy management

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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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