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Intrinsic pentagon defect engineering in multiple spatial-scale carbon frameworks for efficient triiodide reduction

Journal of energy Chemistry 2024年第8期95卷 20-28,I0002页

作者： Siyi Hou Xuedan Song Chang Yu Jiangwei Chang Yiwang Ding Yingbin Liu Xiubo Zhang Weizhe Liu Jieshan Qiu State Key lab of Fine Chemicals Liaoning Key Lab for Energy Materials and Chemical EngineeringFrontier Science Center for Smart MaterialsSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina Liaoning Key lab for energy materials and Chemical Engineering Frontier Science Center for Smart MaterialsSchool of ChemistryDalian University of TechnologyDalian 116024LiaoningChina State Key laboratory of Chemical Resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Intrinsic topological defect engineering has been proven as a promising strategy to elevate the electrocatalytic activity of carbon ***,the controllable construction of high-density and specific topological defects in carbon frameworks to reveal the relationship between reactivity and defect structure remains a challenging ***,the intrinsic pentagon carbon sites that can favor electron overflow and enhance their binding affinity towards the intermediates of catalytic reaction are firstly presented by the work function and the p-band center *** experimentally verify this,the cage-opening reaction of fullerene is proposed and utilized for synthesizing carbon quantum dots with specific pentagon configuration(CQDs-P),subsequently utilizing CQDs-P to modulate the micro-scale defect density of three-dimensional reduced graphene oxide(rGO)viaπ-π*** multiple spatial-scale rGO-conjugated CQDs-P structure simultaneously possesses abundant pentagon and edge defects as catalytic active sites and long-range-orderedπelectron delocalization system as conductive *** defects-rich CQDs-P/rGO-4 all-carbon-based catalyst exhibits superb catalytic activity for triiodide reduction reaction with a high photoelectric conversion efficiency of 8.40%,superior to the Pt reference(7.97%).Theoretical calculations suggest that pentagon defects in the carbon frameworks can promote charge transfer and modulate the adsorption/dissociation behavior of the reaction intermediates,thus enhancing the electrocatalytic activity of the *** work confirms the role of intrinsic pentagon defects in catalytic reactions and provides a new insight into the synthesis of defects-rich carbon catalysts.

关键词： Defect engineering Pentagon carbon Carbon quantum dots Electrocatalytic activity Triiodide reduction

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An effective'salt in dimethyl sulfoxide/water'electrolyte enables high-voltage supercapacitor operated at-50℃

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Journal of energy Chemistry 2024年第6期93卷 361-367,I0009页

作者： Yingbin Liu Chang Yu Xuedan Song Siyi Hou Shuqin Lan Jinhe Yu Yuanyang Xie Jieshan Qiu State Key lab of Fine Chemicals Frontier Science Center for Smart MaterialsSchool of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina School of Chemistry Frontier Science Center for Smart MaterialsLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina College of Chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Compared with organic electrolytes,aqueous electrolytes exhibit significantly higher ionic conductivity and possess inherent safety features,showcasing unique advantages in ***,challenges remain for low-salt aqueous electrolytes operating at high voltage and low ***,we report a low-salt(0.87 m,m means mol kg^(-1))'salt in dimethyl sulfoxide/water'hybrid electrolyte with non-flammability via hybridizing aqueous electrolyte with an organic co-solvent of dimethyl sulfoxide(hydrogen bond acceptor).As a result,the 0.87 m hybrid electrolyte exhibits enhanced electrochemical stability,a freezing temperature below-50℃,and an outstanding ionic conductivity of 0.52mS cm~(-1)at-50℃.Dimethyl sulfoxide can anchor water molecules through intermolecular hydrogen bond interaction,effectively reinforcing the stability of water in the hybrid ***,the interaction between dimethyl sulfoxide and water molecules diminishes the involvement of water in the generation of ordered ice crystals,finally facilitating the low-temperature performance of the hybrid *** paired with the 0.87 m'salt in dimethyl sulfoxide/water'hybrid electrolyte,the symmetric supercapacitor presents a 2.0 V high operating voltage at 25℃,and can operate stably at-50℃.Importantly,the suppressed electrochemical reaction of water at-50℃further leads to the symmetric supercapacitor operated at a higher voltage of 2.6 *** modification strategy opens an effective avenue to develop low-salt electrolytes for high-voltage and low-temperature aqueous supercapacitors.

关键词： Dimethyl sulfoxide Co-solvent High voltage Low temperature Supercapacitors

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Regulation of pseudographitic carbon domain to boost sodium energy storage

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Nano Research 2024年第6期17卷 5188-5196页

作者： Zhidong Hou Mingwei Jiang Da Lei Xiang Zhang Yuyang Gao Jian-Gan Wang State Key laboratory of Solidification Processing Center for Nano Energy MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical University and Shaanxi Joint Lab of Graphene(NPU)Xi’an 710072China

Hard carbon anode has shown extraordinary potentials for sodium-ion batteries(SIBs)owing to the cost-effectiveness and advantaged ***,the widespread application of hard carbon is still hindered by the insufficient sodium storage capacity and depressed rate property,which are mainly induced by the undesirable pseudographitic ***,we develop a molten-salt-mediated strategy to regulate the pseudographitic structure of hard carbon with suitable interlayer spacing and enlarged pseudographitic domain,which is conducive to the intercalation capacity and diffusion kinetics of sodium ***,the optimized hard carbon anode delivers a high reversible capacity of 320 mAh·g^(−1),along with superior rate property(138 mAh·g−1 at 2 A·g^(−1))and stable cyclability over 1800 ***,the in situ Raman spectroscopic study and full-cell assembly further investigate the sodium storage mechanism and practical implement of obtained hard *** work pioneers a low-cost and effective route to regulate the pseudographitic structure of hard carbon materials for advanced SIBs.

关键词： pseudographitic structure molten salt hard carbon anode sodium-ion batteries

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Heterointerface engineering of assembled CoP_(2) on N-modified carbon as efficient trifunctional electrocatalysts for Zn-Air batteries and overall water splitting

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Nano Research 2024年第5期17卷 3801-3809页

作者： Yan Chen Zhenrui Yang Juan Wang Yun Yang Xuedong He Yang Wang Jiadong Chen Yaqing Guo Xin Wang Shun Wang Huile Jin Wenzhou Key lab of Advanced energy Storage and Conversion Zhejiang Province Key Lab of Leather EngineeringCollege of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Zhejiang Engineering Research Center for Electrochemical energy materials and Devices Institute of New Materials and Industrial TechnologiesWenzhou UniversityWenzhou 325035China School of Chemical and Biomedical Engineering Nanyang Technological UniversitySingapore 637459Singapore

Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective ***,the electronic structure modulation of CoP_(2) supported N-modified carbon(CoP_(2)/NC)has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER).Notably,CoP_(2)/NC-1 catalyst exhibits impressive performance in alkaline media,with an ORR half-wave potential of 0.84 V,as well as OER and HER overpotentials of 290 and 129 mV(at 10 mA·cm^(−2)),*** addition,CoP_(2)/NC-1 produces a power density as high as 172.9 mW·cm^(−2),and excellent reversibility of 100 h at 20 mA·cm^(−2) in home-made Zn-air *** experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP_(2) material significantly enhance the kinetics of ORR,OER,and *** functional theory(DFT)calculations reveal the strong electrons redistribution of CoP_(2) induced by high-density N atoms at the interface,thus optimizing the key intermediates and significantly lower the energy barrier of *** electronic adjustments of CoP_(2) greatly enhance its kinetics of ORR/OER/HER,leading to faster *** study provides profound insights into the specific modification of CoP_(2) by N-doped carbon,enabling the construction of efficient catalysts.

关键词： two-dimensional(2D)carbon metal-organic framework cobalt phosphide zinc air battery water splitting

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Hole-Transporting materials with Rational Combination of Pyridine and Dibenzo[a,c]phenazine as Electron Acceptor for Dopant-Free Perovskite solar Cells

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Chinese Journal of Chemistry 2024年第10期42卷 1100-1106页

作者： Weidong Ling Fei Wu Wentao Yuan Linna Zhu Qianqian Li Zhen Li Hubei Key lab on Organic and Polymeric Opto-Electronic materials Department of ChemistryWuhan UniversityWuhanHubei 430072China Chongqing Key laboratory for Advanced materials and Technologies of Clean energy Faculty of Materials&EnergySouthwest UniversityChongqing400715China TaiKang Center for Life and Medical Sciences Wuhan UniversityWuhanHubei 430072China

Perovskite solar cells(PSCs)have been proven to be a promising option for photovoltaic *** the aim to achieve efficient and stable PSCs,it is essential to explore dopant-free hole-transporting materials(HTMs)with high hole ***,HTMs bearing electron donor(D)-electron acceptor(A)-electron donor(D)structures have been constructed with strong intramolecular charge transfer(ICT)effect,based on rational combination of dibenzo[a,c]phenazine and pyridine as electronic acceptors and anchoring groups to perovskite ***,high hole mobility(7.31×10^(-5) cm^(2)·V^(-1)·s^(-1))and photoelectric conversion efficiency(20.45%)have been achieved by dopant-free DPyP-based *** afforded an efficient way to design HTMs with high hole mobility by adjustment of molecular configurations and electronic property of conjugated systems.

关键词： Perovskite solar cell Charge transfer Donor-acceptor systems energy conversion Hole mobility

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Spatial construction of ultrasmall Pt-decorated 3D spinel oxidemodified N-doped graphene nanoarchitectures as high-efficiency methanol oxidation electrocatalysts

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Rare Metals 2024年第1期43卷 186-197页

作者： Qi Zhang Min-Min Yan Wen-Fa Du Chen-Yu Yin Jian Zhang Lu Yang Yun-Qing Kang Hai-Yan He Hua-Jie Huang College of Mechanics and materials Hohai UniversityNanjing 210098China New energy Technology Engineering lab of Jiangsu Province College of ScienceNanjing University of Posts&Telecommunications(NUPT)Nanjing 210023China International Center for materials Nanoarchitectonics(WPIMANA) National Institute for Materials ScienceTsukuba 305-0044IbarakiJapan

Direct methanol fuel cell technology recently becomes the focus of both academic and engineering circles,which stimulates the exploitation and utilization of advanced electrode catalysts with high activity and long ***,we demonstrate a robust bottom-up approach to the spatial construction of three-dimensional(3D) spinel manganese-cobalt oxide-modified N-doped graphene nanoarchitectures decorated with ultrasmall Pt nanoparticles(Pt/MnCo_(2)O_(4)-NG) via a controllable selfassembly *** incorporation of MnCo_(2)O_(4)nanocrystals provides abundant hydroxyl sources to promote the oxidative removal of CO-like byproducts on Pt sites,while the existence of 3D porous N-doped graphene networks facilitates the transportation of both ions and electrons in the hybrid system,thus giving rise to remarkable synergetic coupling effects during the methanol oxidation ***,the optimized Pt/MnCo_(2)O_(4)-NG nano architecture expres ses exceptional electrocatalytic properties with a large electrochemically active surface area of 99.5 m^(2)·g^(-1),a high mass activity of1508.3 mA·mg^(-1),strong toxicity resistance and reliable long-term durability,which have obvious competitive advantages over those of conventional Pt/carbon black,Pt/carbon nano tube,Pt/graphene,and Pt/N-doped graphene catalysts with the same Pt usage.

关键词： Platinum MnCo_(2)O_(4) 3D graphene Electrocatalysts Methanol oxidation

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Enhancement of–OH content on mechanical properties of antiperovskite solid electrolytes

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Nano Research 2024年第7期17卷 6139-6146页

作者： Zunqiu Xiao Huaying Wang Ningyuan Cai Yutong Li Kejia Xiang Wei Wei Tao Ye Zhongtai Zhang Shitong Wang Zilong Tang State Key lab of New Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China College of New energy Advanced Chemical Engineering and Energy Materials Research CenterChina University of Petroleum(East China)Qingdao 266580China Department of Nuclear Science and Engineering Massachusetts Institute of TechnologyCambridgeMA 02139USA

All-solid-state batteries,renowned for their enhanced safety and high energy density,have garnered broad *** solid electrolytes are highly anticipated for their balanced ***,their high Young’s modulus and inadaptability to volume change during cycling lead to poor contact and eventual battery *** this work,Young’s modulus of Li_(1+x)(OH)_(x)Cl samples is lowered to a level comparable to that of sulfide by regulating the–OH *** the–OH content increases,Young’s modulus of Li_(1+x)(OH)_(x)Cl samples decreases *** may be due to the local aggregation of–OH groups,forming cavities similar to LiOH structure,which reduces the bonding of the *** the premise of high Li-ion conductivity and electrochemical stability,the lowered Young’s modulus improves the contact between the solid electrolyte and the electrodes,forming a strong and stable interfacial layer,thereby improving interfacial and cycling *** symmetrical lithium metal cell shows excellent cycle performance of 600 h,and the assembled LiFePO_(4)|Li_(2.4)(OH)1.4Cl|Li cell shows significantly enhanced cycling endurance with 80%capacity retention after 150 *** work not only emphasizes the crucial importance of Young’s modulus in improving interface issues but also offers innovative approaches to advance the mechanical properties of solid electrolytes.

关键词： mechanical properties -OH content anti-perovskite solid electrolytes Li-ion batteries

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Strategies to advance thermoelectric performance of PbSe and PbS materials

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Rare Metals 2024年第9期43卷 4099-4114页

作者： Zheng-Hao Hou Xin Qian Qiu-Juan Cui Shu-Fang Wang Li-Dong Zhao Shijiazhuang Key laboratory of Low Carbon energy materials College of Chemical EngineeringShijiazhuang University Hebei Key lab of Optic-Electronic Information and materials College of Physics Science and Technology Hebei University School of materials Science and Engineering Beihang University

Thermoelectric materials possess the unique capability to convert thermal energy into electric energy and vice versa, making them promising for waste heat recovery and efficient cooling systems. Currently, extensively investigated thermoelectric materials such as Bi2Te3,PbTe and GeTe exhibit superior thermoelectric properties at room temperature and medium temperature ***, the broad application of these thermoelectric materials has been impeded by the high cost and restricted accessibility of Te and Ge in the earth's crust. Over the past few years, researchers have shown increasing interest in PbSe-and PbS-based materials, primarily attributed to their abundant elemental supply and relatively low costs. The assessment of research progress and a comprehensive overview of optimization strategies in time can significantly contribute to further improving the thermoelectric performance. These strategies include optimizing carrier concentration(aliovalent doping, dynamic doping and defect state), enhancing density-of-state effective mass(band convergence, band flattening and energy filtering effect), optimizing carrier mobility(band sharpening and band alignment) and reducing lattice thermal conductivity(all-scale hierarchical defect structures designing). This systematic summary and analysis provide novel insights and perspectives for the development of thermoelectric materials.

关键词： Carrier concentration

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Negative enthalpy alloys and local chemical ordering:a concept and route leading to synergy of strength and ductility

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National Science Review 2024年第4期11卷 172-184页

作者： Zibing An Tao Yang Caijuan Shi Shengcheng Mao Lihua Wang Ang Li Wei Li Xianmeng Xue Ming Sun Yifan Bai Yapeng He Fuzeng Ren Zhouguang Lu Ming Yan Yang Ren Chain-Tsuan Liu Ze Zhang Xiaodong Han Beijing Key lab of Microstructure and Property of Advanced materials College of Materials Science &Engineering Beijing University of Technology Department of materials Science and Engineering City University of Hong Kong Key laboratory of Partial Acceleration Physics& Technology Institute of High Energy PhysicsChinese Academy of Sciences Department of materials Science &Engineering Southern University of Science and Technology Department of Physics City University of Hong Kong State Key laboratory of Silicon materials Department of Materials Science and Engineering Zhejiang University

Solid solutions are ubiquitous in metals and alloys. Local chemical ordering(LCO) is a fundamental sub-nano/nanoscale process that occurs in many solid solutions and can be used as a microstructure to optimize strength and ductility. However, the formation of LCO has not been fully elucidated, let alone how to provide efficient routes for designing LCO to achieve synergistic effects on both superb strength and ductility. Herein, we propose the formation and control of LCO in negative enthalpy alloys. With engineering negative enthalpy in solid solutions, genetic LCO components are formed in negative enthalpy refractory high-entropy alloys(RHEAs). In contrast to conventional ‘trial-and-error' approaches, the control of LCO by using engineering negative enthalpy in RHEAs is instructive and results in superior strength(1160 MPa) and uniform ductility(24.5%) under tension at ambient temperature, which are among the best reported so far. LCO can promote dislocation cross-slip, enhancing the interaction between dislocations and their accumulation at large tensile strains; sustainable strain hardening can thereby be attained to ensure high ductility of the alloy. This work paves the way for new research fields on negative enthalpy solid solutions and alloys for the synergy of strength and ductility as well as new functions.

关键词： negative enthalpy alloys local chemical ordering strength ductility dislocation

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A novel Tb^(3+) and Eu^(3+) co-doped dual-emitting phosphate K_(3)SrBi(P_(2)O_(7))_(2) phosphor for application in FIR thermometers

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Journal of Rare Earths 2024年第3期42卷 455-463,I0001页

作者： Baochen Wang Shifeng Sun Zeqi Li Zongwang Li Weiwei Lin Chao Zeng Yan-gai Liu Ruiyu Mi School of Chemical and Environmental Engineering Anhui Polytechnic UniversityWuhu241000China State-Province Joint Engineering laboratory of Zeolite Membrane materials Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationInstitute of Advanced MaterialsCollege of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang330022China Beijing Key laboratory of materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral MaterialsSchool of Materials Science and TechnologyChina University of GeosciencesBeijing100083China

Rare earth co-doped phosphor for fluorescence intensity ratio(FIR) thermometer has gained increasing attention in recent years. Herein, the novel Tb^(3+)and Eu^(3+)co-doped K_(3)SrBi(P_(2)O_(7))_(2)(KSBP) phosphate phosphors were reported. The crystal structure of the title phosphor was determined using Rietveld refinement and proved to have a three-dimensional structure. The time-resolved spectroscopy reveals that there is almost no energy transfer between Tb^(3+)and Eu^(3+). More importantly, Tb^(3+)and Eu^(3+)emissions show different thermal quenching behaviors, which claims the potential of this material for application in optical thermometer. The FIR of the typical KSBP:0.02Tb^(3+),0.04Eu^(3+)sample demonstrates a polynomial relationship as a function of temperature and the absolute and relative sensitivity are0.025 K^(-1) and 0.59%/K, respectively. In general, our study reports a novel and potential KSBP:Tb^(3+),Eu^(3+)phosphate phosphor that is promising for use in high-sensitive FIR thermometers.

关键词： Phosphor Thermometer Fluorescence intensity ratio Thermal stability Rare earths

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