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Science China Chemistry 2022年第10期65卷 1903-1910页

作者： Ruiqi Wang Xian Zhang Fuqiang Huang Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Qian Xuesen Laboratory of Space Technology China Academy of Space TechnologyBeijing 100094China State Key Laboratory of High-Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China

The salt-inclusion materials have drawn significant attention for their manifold structural chemistry and novel physical/chemical properties.Herein,two new salt-inclusion chalcohalides,[Cs_(6)Cl][Ga_(5)GeQ_(12)](Q=S,Se),have been discovered via hightemperature flux methods.The two isostructural compounds are constructed by porous[Ga_(5)GeQ_(12)]^(5−)layers with[ClCs_(6)]^(5+)octahedra filled in the holes.The[Ga_(5)GeQ_(12)]^(5−)layer is composed of the honeycomb-like(Ga/Ge)_(18)Q_(42)rings containing(Ga/Ge)_(3)Q_(9)trimer as basic unit.The band gaps of the two compounds are 3.90 and 2.89 eV,respectively.[Cs_(6)Cl][Ga_(5)GeS_(12)]exhibits interesting two-band emission properties which are related to the intermediate-band electronic structure revealed by density functional theory(DFT)calculations.Owing to the porous layered structure,[Cs_(6)Cl][Ga_(5)GeS_(12)]exhibits topological ion exchange ability towards Cd^(2+)ions with the maximum sorption capacity of 250 mg/g and high distribution coefficient(Kd)near 106 mL/g.This work further enriches the structural diversity of salt-inclusion materials and extends their potential application range to ion exchange adsorption.

关键词： heteroanionic compound layered structure two-band emission ion exchange properties

Metal cyanamides: Open-framework structure and energy conversion/storage applications

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Journal of Energy Chemistry 2021年第10期30卷 347-367,I0010页

作者： Bingquan Jia Du Sun Wei Zhao Fuqiang Huang State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Beijing National Laboratory for Molecular Sciences and State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Metal cyanamides are an emerging class of functional materials with potential applications in sustainable energy conversion and storage technologies such as catalysis,supercapacitors,photoluminescence and next-gen batteries.The[NCN]^(2-)as the anion,which is isolobal with[O]^(2-)endows metal cyanamides with similar physicochemical properties as oxides and chalcogenides.Whereas the unique quasI-linear structure and electronic resonance between[N=C=N]^(2-)and[N-C≡N]^(2-)of[NCN]entity bring out superior properties beyond oxides and chalcogenides.In this review,we present research status,challenges,and the recent striking progress on the metal cyanamides in the synthesis and applications.Specifically,the characteristic structures,physicochemical properties,synthetic methods with corresponding merits/demerits and latest applications in energy conversion and storage of cyanamides are summarized.The detailed outlooks for the new compounds design,morphology manipulation and potential applications are also exhibited.

关键词： Metal cyanamides Structure Properties Synthesis Energy applications

[CsCl][GaGeQ](Q = S, Se): two novel porous layered chalcohalides exhibiting two-band emission and ion exchange properties

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Science China Chemistry 2022年

作者： Ruiqi Wang Xian Zhang Fuqiang Huang Qian Xuesen Laboratory of Space Technology China Academy of Space Technology Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular Engineering Peking University State Key Laboratory of High-Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences

The salt-inclusion materials have drawn significant attention for their manifold structural chemistry and novel physical/chemical properties. Herein, two new salt-inclusion chalcohalides, [CsCl][GaGeQ](Q = S, Se), have been discovered via hightemperature flux methods. The two isostructural compounds are constructed by porous [GaGeQ]layers with [ClCs]octahedra filled in the holes. The [GaGeQ]layer is composed of the honeycomb-like(Ga/Ge)Qrings containing(Ga/Ge)Qtrimer as basic unit. The band gaps of the two compounds are 3.90 and 2.89 eV, respectively. [CsCl][GaGeS] exhibits interesting two-band emission properties which are related to the intermediate-band electronic structure revealed by density functional theory(DFT) calculations. Owing to the porous layered structure, [CsCl][GaGeS] exhibits topological ion exchange ability towards Cdions with the maximum sorption capacity of 250 mg/g and high distribution coefficient(Kd) near 10~6 mL/g. This work further enriches the structural diversity of salt-inclusion materials and extends their potential application range to ion exchange adsorption.

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In-situ construction of PDOL electrolyte with dual-reinforced stable interface for high-voltage lithium metal batteries

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Science China Chemistry 2024年第5期67卷 1664-1671页

作者： Yingkang Wu Yuzhou Bai Wujie Dong Xue Wang Wenqin Ma Fuqiang Huang State Key Lab of Metal Matrix Composites School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China School of Physical Science and Technology Shanghai Tech UniversityShanghai 201210China Shanghai Institute of Ceramics Chinese Academy of SciencesShanghai 200050China

In-situ polymerized electrolytes significantly enhance the interfacial compatibility of lithium metal batteries(LMBs). Typically,in-situ polymerized 1,3-dioxolane(PDOL) exhibits low interfacial resistance, yet still suffers from low ionic conductivity and a narrow electrochemical stability window(ESW). Here, an ultra-stable PDOL-based polymer electrolyte is developed by incorporating plasticizers of tetramethylene sulfone(TMS) and fluorinated ethylene carbonate(FEC) into the 3D cross-linked network, achieving a significant enhancement in the transport capacity and efficiency of Li-ion. The ionic conductivity reaches3.63×10^(-4)S cm^(-1)even at room temperature, and the transference number(tLi^(+)) is even higher at 0.85. Furthermore, the ESW of this electrolyte can be increased to 4.5 V with the addition of TMS, which forms a thin and robust antioxidant cathode-electrolyte interface(CEI) on the surface of high-voltage LiCoO_(2). FEC generates an inorganic-rich solid-electrolyte interface(SEI) on the Li anode, which effectively inhibits the growth of lithium dendrites. Benefiting from the aforementioned advantages, the highvoltage lithium metal battery demonstrates outstanding long-cycle stability, with 93.2% capacity retention after 200 cycles. This work offers a straightforward and accessible method for the practical implementation of high energy density in-situ polymerized solid-state LMBs.

关键词： solid polymer electrolyte in-situ polymerization PDOL high-voltage LMBs

SiO2 stabilizes electrochemically active nitrogen in few-layer carbon electrodes of extraordinary capacitance

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Journal of Energy Chemistry 2020年第10期29卷 179-188页

作者： Feng Xu Tianquan Lin Jian huang I-Wei Chen Fuqiang Huang State Key Laboratory of High Performance Ceramics and Superfine Microstructure.Shanghai Institute of Ceramics Chinese Academy of SciencesShanghai 200050China University of Chinese Academy of Sciences 19 Yuquan RoadBeijing 100049China Department of Materials Science and Engineering University of PennsylvaniaPhiladelphiaPA 19104USA College of Chemistry and Molecular Engineering Peking UniversityBeijing 100871China

Pyrrolic and pyridinic N dopants can dramatically increase the electrochemical activities of carbon and conducting polymers.Although N-doped conducting polymers suffer from rapid degradation,their carbon counterpart of extraordinary capacitance has remarkable rate performance and cycling endurance thanks to carbon’s excellent electrical conductivity.But high nitrogen content and high electrical conductivity are difficult to achieve in a high-surface-area carbon,because the high chemical vapor deposition(CVD)temperature required for obtaining high conductivity also destabilizes under-coordinated pyrrolic and pyridinic nitrogen and tends to lower the surface area.Here we resolve this dilemma by using SiO2 as an effective N-fixation additive,which stabilizes the N-rich nano few-layer sp2-carbon construct in1000℃CVD.This enables a scalable sol-gel/CVD fabrication process for few-layer carbon electrodes of extraordinary capacitance(690 F g^-1).The electrodes have excellent rate performance and can maintain90%of their initial capacitance after 30,000 cycles,thus potentially suitable for practical applications.

关键词： Electrochemical capacitors Carbon electrodes Extraordinary capacitance SiO2 stabilized nitrogen

High‑Entropy Layered Oxide Cathode Enabling High‑Rate for Solid‑State Sodium‑Ion Batteries

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Nano-Micro Letters 2024年第1期16卷 160-171页

作者： Tianxun Cai Mingzhi Cai Jinxiao Mu Siwei Zhao Hui Bi Wei Zhao Wujie Dong Fuqiang Huang State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050People’s Republic of China State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871People’s Republic of China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049People’s Republic of China Zhongke Institute of Strategic Emerging Materials Yixing 214213JiangsuPeople’s Republic of China

Na-ion O3-type layered oxides are prospective cathodes for Na-ion batteries due to high energy density and low-cost.Nevertheless,such cathodes usually suffer from phase transitions,sluggish kinetics and air instability,making it difficult to achieve high performance solid-state sodium-ion batteries.Herein,the high-entropy design and Li doping strategy alleviate lattice stress and enhance ionic conductivity,achieving high-rate performance,air stability and electrochemically thermal stability for Na_(0.95)Li_(0.06)Ni_(0.25)Cu_(0.05)Fe_(0.15)Mn_(0.49)O_(2).This cathode delivers a high reversible capacity(141 mAh g^(−1)at 0.2C),excellent rate capability(111 mAh g^(−1)at 8C,85 mAh g^(−1)even at 20C),and long-term stability(over 85%capacity retention after 1000 cycles),which is attributed to a rapid and reversible O3–P3 phase transition in regions of low voltage and suppresses phase transition.Moreover,the compound remains unchanged over seven days and keeps thermal stability until 279℃.Remarkably,the polymer solid-state sodium battery assembled by this cathode provides a capacity of 92 mAh g^(−1)at 5C and keeps retention of 96%after 400 cycles.This strategy inspires more rational designs and could be applied to a series of O3 cathodes to improve the performance of solid-state Na-ion batteries.

关键词： High-entropy High-rate performance Li-TM interaction Air stability O3 layered oxide cathode

Unlocking efficient energy storage via regulating ion and electron-active subunits:an(SbS)_(1.15)TiS_(2)superlattice for large and fast Na^(+)storage

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Science China Chemistry 2024年第1期67卷 336-342页

作者： Baixin Peng Tianxun Cai Shaoning Zhang Yuqiang Fang Zhuoran Lv Yusha Gao Fuqiang Huang State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China School of Physical Science and Technology ShanghaiTech UniversityShanghai 200031China Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Alloying-type metal sulfides with high sodiation activity and theoretical capacity are promising anode materials for high energy density sodium ion batteries.However,the large volume change and the migratory and aggregation behavior of metal atoms will cause severe capacity decay during the charge/discharge process.Herein,a robust and conductive TiS_(2)framework is integrated with a high-capacity SbS layer to construct a single phase(SbS)_(1.15)TiS_(2)superlattice for both high-capacity and fast Na^(+)storage.The metallic TiS_(2)sublayer with high electron activity acts as a robust and conductive skeleton to buffer the volume expansion caused by conversion and alloying reaction between Na+and SbS sublayer.Hence,high capacity and high rate capability can be synergistically realized in a single phase(SbS)_(1.15)TiS_(2)superlattice.The novel(SbS)_(1.15)TiS_(2)anode has a high charge capacity of 618 mAh g^(-1)at 0.2 C and superior rate performance and cycling stability(205 mAh g^(-1)at 35 C after 2,000 cycles).Furthermore,in situ and ex situ characterizations are applied to get an insight into the multi-step reaction mechanism.The integrity of robust Na-Ti-S skeleton during(dis)charge process can be confirmed.This superlattice construction idea to integrate the Na^(+)-active unit and electron-active unit would provide a new avenue for exploring high-performance anode materials for advanced sodium-ion batteries.

关键词： (SbS)_(1.15)TiS_(2) sulfides sodium ion battery superlattice fast-charging

Multiple Nanoparticles Coupling Strategy for Enhancing Optical Filter Performance of Spectral Splitter Used in Photovoltaic/Thermal System

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Journal of Thermal Science 2024年第1期33卷 368-382页

作者： LIANG Huaxu huang Xin WANG fuqiang CHENG Ziming DONG Yan School of Energy Science and Engineering Harbin Institute of TechnologyHarbin 150001China School of New Energy Harbin Institute of Technology at WeihaiWeihai 264209China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore

Selective absorptive nanofluid can pre-absorb certain sunlight wavelength that cannot be used by PV and transmits remaining sunlight to the surface of PV,which can decouple PV from the thermal receiver spatially.In order to improve the harvesting of electricity and high-temperature thermal nanofluid,it is important to design an optimal optical filter window(transmit sunlight with wavelengths of 732-1067 nm to the surface of the photovoltaic cell and absorb the remaining sunlight).However,designing optimal optical filter is facing following challenges:(1) inherently narrow selective absorptivity property of single nanoparticle;(2) simplified numerical calculation method calculating transmittance;(3) ignoring the shape of the nanoparticle.In this study,the idea of using multiple nanoparticles coupling effect to design an optical filter is proposed,which can superimpose the narrow absorption bandwidth of different nanoparticles to obtain a wide absorption bandwidth of the whole system.In addition,an improved transmission method considering light-matter interaction at air/vessel and liquid/vessel interfaces is adopted to compute the transmittance.The results calculated by improved transmission method are more accurate than widely used traditional Lambert-Beer law,which is verified by experimental test.Furthermore,the effect of nanoparticle shape on spectral transmittance is also investigated,which shows that spiny Ag can approximately extend absorbance from 400 nm to 600 nm compared to nanosphere silver.Finally,the results show that optical filter efficiency of nanofluids with multiple nanoparticles coupling(Ag,spiny Ag,ZnO,ITO) can reached up to 35%.

关键词： solar energy PV/T nanofluid optimal optical filter radiative transfer spectral splitting

One-Step High-Temperature-Synthesized Single-Atom Platinum Catalyst for Efficient Selective Hydrogenation

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Research 2020年第1期2020卷 1746-1755页

作者： Qingyuan Bi Xiaotao Yuan Yue Lu Dong Wang Jian huang Rui Si Manling Sui Fuqiang Huang State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Institute of Microstructure and Properties of Advanced Materials Beijing University of TechnologyBeijing 100124China Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201800China

Although single-atom catalysts significantly improve the atom utilization efficiency,the multistep preparation procedures are complicated and difficult to control.Herein,we demonstrate that one-step in situ synthesis of the single-atom Pt anchored in single-crystal MoC(Pt_(1)/MoC)by using facile and controllable arc-discharge strategy under extreme conditions.The high temperature(up to 4000℃)provides the sufficient energy for atom dispersion and overall stability by forming thermodynamically favourable metal-support interactions.The high-temperature-stabilized Pt1/MoC exhibits outstanding performance and excellent thermal stability as durable catalyst for selective quinoline hydrogenation.The initial turnover frequency of 3710 h^(-1)is greater than those of previously reported samples by an order of magnitude under 2 MPa H_(2)at 100℃.The catalyst also shows broad scope activity toward hydrogenation containing unsaturated groups of C=C,C=N,and C=O.The facile,one-step,and fast arc-discharge method provides an effective avenue for single-atom catalyst fabrication that is conventionally challenging.

关键词： catalyst hydrogenation facile

Manipulating oxygenate adsorption on N-doped carbon by coupling with CoSn alloy for bifunctional oxygen electrocatalyst

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Green Energy & Environment 2023年第5期8卷 1417-1428页

作者： Chenlong Dong Xilin Zhang Shaoning Zhang Siwei Zhao Xueyu Lin Xin Wang Yajing Zhang Fuqiang Huang Tianjin Key Laboratory for Photoelectric Materials and Devices School of Materials Science and EngineeringTianjin University of TechnologyTianjin300384China Beijing National Laboratory for Molecular Sciences and State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China School of Physics Henan Normal UniversityXinxiang453007China State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai200050China College of Chemistry Zhengzhou UniversityZhengzhou450001China

Highly active bifunctional oxygen electrocatalysts accelerate the development of high-performance Zn-air battery,but suffer from the mismatched activities of oxygen evolution reaction(OER)and oxygen reduced reaction(ORR).Herein,highly integrated bifunctional oxygen electrocatalysts,cobalt-tin alloys coated by nitrogen doped carbon(CoSn@NC)are prepared by MOFs-derived method.In this hybrid catalyst,the binary CoSn nanoalloys mainly contribute to highly active OER process while the Co(or Sn)-N-C serves as ORR active sites.Rational interaction between CoSn and NC donates more rapid reaction kinetics than Pt/C(ORR)and IrO_(2)(OER).Such CoSn@NC holds a promise as air-cathode electrocatalyst in Zn-air battery,superior to Pt/C+IrO_(2)catalyst.First-principles calculations predict that CoSn alloys can upgrade charge redistribution on NC and promote the transfer to reactants,thus optimizing the adsorption strength of oxygen-containing intermediates to boost the overall reactivity.The tuning of oxygenate adsorption by interactions between alloy and heteroatom-doped carbon can guide the design of bifunctional oxygen electrocatalysts.

关键词： CoSn alloy Oxygenate adsorption Nitrogen-doped carbon Bifunctional catalyst Zn-air battery