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Polyoxometalates for continuous power generation by atmospheric humidity

Nano Research 2024年第3期17卷 1875-1885页

作者： Tuo Ji Weilin Chen zhenhui kang Liming Zhang Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Northeast Normal UniversityChangchun 130024China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&Devices DepartmentSoochow UniversitySuzhou 215123China Macao Institute of Materials Science and Engineering Macao University of Science and TechnologyTaipaMacao 999078China Institute of Functional State Key Laboratory of Luminescence and Applications Changchun Institute of OpticsFine Mechanics and PhysicsChinese Academy of SciencesChangchun 130033China

Atmospheric humidity is a sustainable low-value energy widely existing in natural environment,which is a promising candidate to solve the noncontinuous and low efficiency of low-value energy power generation.Here the mono-substituted Dawson-type polyoxometalates are constructed to be highly dispersed organic ammonium-polyoxoanion clusters and are assembled into thin films power generators with micropores,working in atmospheric humidity.The optimal polyoxometalates generator with the thickness of 7.2μm and the area of 0.36 cm^(2) produces a voltage of 0.68 V and a current density of 19.5μA·cm^(-2) under simulated natural environment,and works continuously and stably under almost all-natural environments(humidity 10%–90%).The highly dispersed polyoxometalate nanoclusters can form microporous in polyoxometalate films to effectively absorb atmospheric humidity and spontaneously form distribution gradient of water,which is the structural basis of power generation.The continuous power generation may be maintained by the effective adsorption and utilization of H_(2)O,the huge electrostatic field of organic ammonium-polyoxoanion clusters,and the reasonably designed polyoxometalates containing inorganic small ions with high mobility.It is the first humidity generator designed with polyoxometalates,which may provide a new research direction for polyoxometalates in sustainable utilization of low-value energy.

关键词： atmospheric humidity continuous power generations nanomaterials polyoxoanions polyoxometalates

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Construction of ZnO@CDs@Co_(3)O_(4) sandwich heterostructure with multi-interfacial electron-transfer toward enhanced photocatalytic CO_(2) reduction

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Chinese Chemical Letters 2024年第4期35卷 147-152页

作者： Xiuzheng Deng Yi Ke Jiawen Ding Yingtang Zhou Hui Huang Qian Liang zhenhui kang Advanced Catalysis and Green Manufacturing Collaborative Innovation Center CNPC-CZU Innovation AllianceSchool of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control National Engineering Research Center for Marine AquacultureMarine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316004China

Photocatalytic conversion of CO_(2) into small-molecule chemical feedstocks can meet the growing demand for energy and alleviate the global warming. Herein, a p-n ZnO@CDs@Co_(3)O_(4) heterojunction with sandwich structure was constructed by calcination method of self-assembled ZIF-8@CDs@ZIF-67. The ZnO@CDs@Co_(3)O_(4) with well-defined interfacial structure exhibited the significantly enhanced photocatalytic CO_(2) reduction activity, and the optimal catalyst indicated the(CO + CH_(4)) evolution rate of 214.53μmol g^(-1)h^(-1) under simulated solar light, which was superior to ZnO, Co_(3)O_(4) and binary ZnO@Co_(3)O_(4).The internal cavity, exposed active sites, multiple interfaces and constructed p-n heterojunction can facilitate the light harvesting and photoexcited electron transfer. Besides, after introduction of CDs placed in the middle layer between ZnO and Co_(3)O_(4), CDs with excellent photoelectric property further promoted charge separation and migration. This work represents an appealing strategy to construct well-defined photocatalysts for boosting CO_(2) photoreduction.

关键词： Metal-organic framework Photocatalytic CO_(2) reduction Carbon dots p-n heterojunction Sandwich heterostructure

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The advanced multi-functional carbon dots in photoelectrochemistry based energy conversion

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International Journal of Extreme Manufacturing 2022年第4期4卷 1-18页

作者： Yunjie Zhou Fan Liao Yang Liu zhenhui kang Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow University199 Ren'ai RoadSuzhouJiangsu 215123People's Republic of China Macao Institute of Materials Science and Engineering(MIMSE) MUST-SUDA Joint Research Center for Advanced Functional MaterialsMacao University of Science and TechnologyTaipaMacao 999078People's Republic of China

Carbon dots(CDs),as a unique zero-dimensional member of carbon materials,have attracted numerous attentions for their potential applications in optoelectronic,biological,and energy related fields.Recently,CDs as catalysts for energy conversion reactions under multi-physical conditions such as light and/or electricity have grown into a research frontier due to their advantages of high visible light utilization,fast migration of charge carriers,efficient surface redox reactions and good electrical conductivity.In this review,we summarize the fabrication methods of CDs and corresponding CD nanocomposites,including the strategies of surface modification and heteroatom doping.The properties of CDs that concerned to the photo-and electro-catalysis are highlighted and detailed corresponding applications are listed.More importantly,as new non-contact detection technologies,transient photo-induced voltage/current have been developed to detect and study the charge transfer kinetics,which can sensitively reflect the complex electron separation and transfer behavior in photo-/electro-catalysts.The development and application of the techniques are reviewed.Finally,we discuss and outline the major challenges and opportunities for future CD-based catalysts,and the needs and expectations for the development of novel characterization technologies.

关键词： carbon dots photoelectrochemical properties photocatalysis electrocatalysis transient photo-induced voltage transient photo-induced current

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Layered double hydroxide nanosheets activate CsPbBr_(3) nanocrystals for enhanced photocatalytic CO_(2) reduction

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Nano Research 2022年第7期15卷 5953-5961页

作者： Shuang Zhao Qian Liang Zhongyu Li Hong Shi Zhenyu Wu Hui Huang zhenhui kang Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology School of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China Institute of Functional Nano and Soft Materials Laboratory(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Macao Institute of Materials Science and Engineering Macao University of Science and TechnologyTaipa 999078MacaoChina Institute of Advanced Materials Northeast Normal UniversityChangchun 130024China

Halide perovskite nanocrystals are potential catalysts for CO_(2) photoreduction,while,the strong radiative recombination and insufficient stability limit their catalytic performance and application.Herein,we report that layered double hydroxide nanosheets activate CsPbBr_(3) nanocrystals(CLDH)for enhanced photocatalytic CO_(2) reduction.These CLDH heterojunctions show the remarkably enhanced CO_(2) photoreduction performance;without cocatalyst and sacrificial agent,the average electron consumption rate of CLDH(49.16μmol·g^(−1)·h^(−1))is approximately 3.7 times higher than that of pristine CsPbBr_(3).Also,CLDH catalyst exhibits a robust stability after ten cycles over 30 h.

关键词： CsPbBr_(3) NiAl-LDH CO_(2)reduction Z-scheme photocatalysis

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Immobilization of Oxyanions on the Reconstructed Heterostructure Evolved from a Bimetallic Oxysulfide for the Promotion of Oxygen Evolution Reaction

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Nano-Micro Letters 2023年第10期15卷 547-564页

作者： Kai Yu Hongyuan Yang Hao Zhang Hui Huang Zhaowu Wang zhenhui kang Yang Liu Prashanth W.Menezes Ziliang Chen Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon‑Based Functional Materials and DevicesJoint International Research Laboratory of Carbon‑Based Functional Materials and DevicesSoochow UniversitySuzhou 215123People’s Republic of China Department of Chemistry:Metalorganics and Inorganic Materials Technical University of BerlinStrase Des 17 Juni 135.Sekr.C210623 BerlinGermany Materials Chemistry Group for Thin Film Catalysis–CatLab Helmholtz-Zentrum Berlin fur Materialien und EnergieAlbert‑Einstein‑Str.1512489 BerlinGermany School of Physics and Engineering Longmen LaboratoryHenan University of Science and TechnologyLuoyang 471023People’s Republic of China

Efficient and durable oxygen evolution reaction(OER)requires the electrocatalyst to bear abundant active sites,optimized electronic structure as well as robust component and mechanical stability.Herein,a bimetallic lanthanum-nickel oxysulfide with rich oxygen vacancies based on the La_(2)O_(2)S prototype is fabricated as a binder-free precatalyst for alkaline OER.The combination of advanced in situ and ex situ characterizations with theoretical calculation uncovers the synergistic effect among La,Ni,O,and S species during OER,which assures the adsorption and stabilization of the oxyanion SO_(4)^(2-)onto the surface of the deeply reconstructed porous heterostructure composed of confining Ni OOH nanodomains by La(OH)_3 barrier.Such coupling,confinement,porosity and immobilization enable notable improvement in active site accessibility,phase stability,mass diffusion capability and the intrinsic Gibbs free energy of oxygen-containing intermediates.The optimized electrocatalyst delivers exceptional alkaline OER activity and durability,outperforming most of the Ni-based benchmark OER electrocatalysts.

关键词： Lanthanum-nickel oxysulfide Rare earth metal Immobilization of oxyanions Structural reconstruction Oxygen evolution catalysis

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Efficient hydrogen peroxide production enabled by exploring layered metal telluride as two electron oxygen reduction reaction electrocatalyst

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Journal of Energy Chemistry 2023年第12期87卷 247-255,I0007页

作者： Yingming Wang Hongyuan Yang Zhiwei Liu Kui Yin Zhaowu Wang Hui Huang Yang Liu zhenhui kang Ziliang Chen Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-based Functional Materials and DevicesJoint International Research Laboratory of Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123JiangsuChina School of Physics and Engineering Longmen Laboratory Henan University of Science and TechnologyLuoyang 471023HenanChina Macao Institute of Materials Science and Engineering(MIMSE) MUST-SUDA Joint Research Center for Advanced Functional MaterialsMacao University of Science and TechnologyTaipa 999078MacaoChina Suzhou Weimu Intelligent System Co. Ltd.Suzhou 215123JiangsuChina

It is of great interest to develop the novel transition metal-based electrocatalysts with high selectivity and activity for two electron oxygen reduction reaction(2e^(-) ORR).Herein,the nickel ditelluride(NiTe_(2)) with layered structure was explored as the 2e^(-) ORR electrocatalyst,which not only showed the highest 2e^(-) selectivity more than 97%,but also delivered a slight activity decay after 5000 cycles in alkaline media.Moreover,when NiTe_(2) was assembled as the electrocatalyst in H-type electrolyzer,the on-site yield of H_(2)O_(2) could reach up to 672 mmol h^(-1)g^(-1) under 0.45 V vs.RHE.Further in situ Raman spectra,theoretical calculation and post microstructural analysis synergistically unveiled that such a good 2e^(-) ORR performance could be credited to the intrinsic layered crystal structure,the high compositional stability,as well as the electron modulation on the active site Ni atoms by neighboring Te atoms,leading to the exposure of active sites as well as the optimized adsorption free energy of Ni to –OOH.More inspiringly,such telluride electrocatalyst has also been demonstrated to exhibit high activity and selectivity towards 2e^(-) ORR in neutral media.

关键词： Transition metal telluride Oxygen reduction reaction Charge polarization Activity and selectivity Hydrogen peroxide

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Carbon dots regulate the interface electron transfer and catalytic kinetics of Pt-based alloys catalyst for highly efficient hydrogen oxidation

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Journal of Energy Chemistry 2022年第3期31卷 61-67,I0003页

作者： Jie Wu Yunjie Zhou Haodong Nie Kaiqiang Wei Hui Huang Fan Liao Yang Liu Mingwang Shao zhenhui kang Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123JiangsuChina Macao Institute of Materials Science and Engineering Macao University of Science and TechnologyTaipa 999078Macao SARChina

The regulation of interface electron-transfer and catalytic kinetics is very important to design the efficient electrocatalyst for alkaline hydrogen oxidation reaction(HOR).Here,we show the Pt-Ni alloy nanoparticles(PtNi_(2))have an enhanced HOR activity compared with single component Pt catalyst.While,the interface electron-transfer kinetics of PtNi_(2)catalyst exhibits a very wide electron-transfer speed distribution.When combined with carbon dots(CDs),the interface charge transfer of PtNi_(2)-CDs composite is optimized,and then the PtNi_(2)-5 mg CDs exhibits about 2.67 times and 4.04 times higher mass and specific activity in 0.1 M KOH than that of 20%commercial Pt/C.In this system,CDs also contribute to trapping H^(+)and H_(2)O generated during HOR,tuning hydrogen binding energy(HBE),and regulating interface electron transfer.This work provides a deep understanding of the interface catalytic kinetics of Pt-based alloys towards highly efficient HOR catalysts design.

关键词： Pt-based alloys Carbon dots Interface electron transfer Interface catalytic kinetics Hydrogen oxidation reaction

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Chiral carbon dots from glucose by room temperature alkaliassisted synthesis for electrocatalytic oxidation of tryptophan enantiomers

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Nano Research 2023年第7期16卷 8929-8936页

作者： Mengling Zhang Xing Fan Xin Du Yurong Ma Xiting Wang Hui Huang Yang Liu Youyong Li zhenhui kang Macao Institute of Materials Science and Engineering(MIMSE) MUST-SUDA Joint Research Center for Advanced Functional MaterialsMacao University of Science and TechnologyTaipaMacao 999078China Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-based Functional Materials and DevicesJoint International Research Laboratory of Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123China Research Center for Carbon-based Electronics and Key Laboratory for the Physics and Chemistry of Nanodevices School of ElectronicsPeking UniversityBeijing 100871China

Chiral catalysis is one of the most direct and effective approach to obtain pure optical enantiomers.Chiral carbon dots(CDs)as carbon-based chiral catalysts show great potential in chiral catalysis.Herein,we report a facile one step base-catalyzed aldol condensation to fabricate the chiral CDs from glucose at ambient temperature and pressure.The formation of chiral CDs involves the processes of isomerization and aldol condensation.These chiral CDs have been demonstrated that they have selective capacity for electrocatalytic oxidization of tryptophan enantiomers.L type of CDs(LCDs)is more likely to catalyze L-tryptophan(Trp)than D-Trp with the selective factor(I_(L)/I_(D))of 1.60,whereas the D type of CDs(DCDs)tends to catalyze D-Trp(I_(L)/I_(D):0.63).Theoretical calculations combined with various contrast experiments(temperature and pH)demonstrate that the selectively electrocatalytic capacity of chiral CDs toward Trp isomers is due to the different hydrogen-bond interactions between chiral CDs and Trp.

关键词： chiral carbon dots synthesis mechanism electrocatalysis chiral catalysis

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Highly crystalline core dominated the catalytic performance of carbon dot for cyclohexane to adipic acid reaction

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Nano Research 2022年第8期15卷 7662-7669页

作者： Xiao Wang Wenyi Bian Tianyang Zhang Yajie Zhao Mingwang Shao Haiping Lin Yang Liu Hui Huang zhenhui kang Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Macao Institute of Materials Science and Engineering(MIMSE) MUST-SUDA Joint Research Center for Advanced Functional MaterialsMacao University of Science and TechnologyTaipa 999078MacaoChina School of Physics and Information Technology Shaanxi Normal UniversityXi’an 710062China

Carbon dots(CDs)have uniquely structural,physicochemical and photochemical properties,suggesting a promising platform for catalysis applications.The in-depth understanding of the structure-activity relationship in the CDs-based catalyst system needs to know the effect of the crystalline core on their catalytic performance.The efficient catalytic oxidation of cyclohexane is an urgent challenge in current chemical industry,in which,adipic acid(AA)plays an important role in industry for synthesis of nylon6 and nylon-66.Here,we fabricated the pristine CDs by electrochemical etching graphite rod method and derived CDs with high crystalline core(CD-600,CD-800,and CD-1100)through a thermal treatment method in tube furnace.Furthermore,these CDs performed an outstanding catalytic performance for one-step synthesis of AA from cyclohexane.With the help of machine learning(ML),the deep correlations between features(structures of CDs,catalytic conditions)and catalytic performances were investigated by XGBoost(XGB)model.Then under the optimization and prediction of XGB,it was found that high crystalline core preceded the other features and CD-1100 could get the best conversion of 30.696%and selectivity to AA of 92.52%at reaction conditions of 130℃,1.5 MPa,and 10 h.This work pioneered the application of ML in industrial issues and demonstrated a comprehensive understanding on CDs as catalyst to realize one-step synthesis of AA.

关键词： adipic acid carbon dots machine learning catalytic performances crystalline core

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Fe-doped SnO_(2) nanosheet for ambient electrocatalytic nitrogen reduction reaction

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Nano Research 2022年第7期15卷 6026-6035页

作者： Yaxi Li Yixian Liu Xiang Liu Yunliang Liu Yuanyuan Cheng Peng Zhang Peiji Deng Jiujun Deng zhenhui kang Haitao Li Institute for Energy Research School of Chemistry and Chemical EngineeringJiangsu UniversityZhenjiang 212013China Institute of Medicine&Chemical Engineering Zhenjiang CollegeZhenjiang 212000China Key Laboratory for Water Quality and Conservation of the Pearl River Delta Ministry of EducationInstitute of Environmental Research at Greater BayGuangzhou UniversityGuangzhou 510006China School of Physics The University of SydneySydneyNew South Wales 2006Australia Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-based Functional Materials and DevicesSoochow UniversitySuzhou 215123China

Ammonia plays a vital role in the development of modern agriculture and industry.Compared to the conventional Haber–Bosch ammonia synthesis in industry,electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising and environmental friendly strategy to synthesize ammonia.Here,inspired by biological nitrogenase,we designed iron doped tin oxide(Fe-doped SnO_(2))for nitrogen reduction.In this work,iron can optimize the interface electron transfer and improve the poor conductivity of the pure SnO_(2),meanwhile,the synergistic effect between iron and Sn ions improves the catalyst activity.In the electrocatalytic NRR test,Fe-doped SnO_(2) exhibits a NH_(3) yield of 28.45μg·h^(−1)·mgcat^(−1),which is 2.1 times that of pure SnO_(2),and Faradaic efficiency of 6.54%at−0.8 V vs.RHE in 0.1 M Na_(2)SO_(4).It also shows good stability during a 12-h long-term stability test.Density functional theory calculations show that doped Fe atoms in SnO_(2) enhance catalysis performance of some Sn sites by strengthening N–Sn interaction and lowering the energy barrier of the rate-limiting step of NRR.The transient photovoltage test reveals that electrons in the low-frequency region are the key to determining the electron transfer ability of Fe-doped SnO_(2).

关键词： electrocatalyst nitrogen reduction reaction Fe-doped SnO_(2)

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