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Engineering versatile Au-based catalysts for solar-to-fuel conversion

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能源化学:英文版 2023年第8期83卷 341-362,I0010页

作者： Chunhua Wang Hongwen Zhang Feili Lai Zhirun Xie y.n hau ng Bo Weng Xuejiao Wu yuhe Liao Department of Chemistry KU LeuvenCelestijinenlaan 200F3001 LeuvenBelgium cMACS Department of Microbial and Molecular SystemsKU LeuvenCelestijnenlaan 200F3001 LeuvenBelgium School of Energy and Environment City University of Hong Kong83 Tat Chee AvenueKowloonHong Kong 999077China Centre for Sustainable Catalysis and Engineering Faculty of Bioscience EngineeringKU Leuven3001 LeuvenBelgium Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640GuangdongChina

Gold(Au) nanostructures(nSs) have been widely employed as cocatalysts to improve the photoactivity of semiconductor materials, while a systematic summary of the engineering approaches of Au nSs to maximize the solar-to-fuel conversion efficiency is still lacking. In this review, the recently developed strategies for elevating the overall photocatalytic performance of Au-based catalysts and the deep physical chemistry mechanisms are highlighted. Firstly, the synthetic approaches of Au nSs are summarized, followed by an elaboration on their multiple functions in improving photoactivity. Afterward, modification strategies of Au nSs used to enhance the photocatalytic efficiency of Au-semiconductor composites,including controlling the Au nSs morphology, size, crystal phase, defect engineering, alloy.ng with different metals, modulating interfacial interaction, and introducing an external field, are summarized and discussed independently. Additionally, advanced characterization techniques that can provide insights into the charge dynamics of the photocatalysts are introduced. Finally, we share our opinion on the challenges and outline potentially promising opportunities and directions for efficient Au-based photocatalysis research moving forward. We sincerely look forward to this review can deliver insightful views to design efficient Au-based photocatalysts and spur certain innovations to other metal-based catalysts.

关键词： Au nanostructures Modification strategies Semiconductor Photocatalysis Solar-to-fuel conversion

FeCo alloy.n-doped graphitized carbon as an efficient cocatalyst for enhanced photocatalytic H2 evolution by inducing accelerated charge transfer

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Journal of Energy Chemistry 2021年第1期30卷 92-101,I0004页

作者： Sibo Chen y.n hau ng Jihai Liao Qiongzhi Gao Siyuan y.ng Feng Peng Xinhua Zhong yueping Fang Shengsen Zhang Key Laboratory for Biobased Materials and Energy of Ministry of Education College of Materials and EnergySouth China Agricultural UniversityGuangzhou 510643GuangdongChina Guangdong Laboratory for Lingnan Modern Agriculture Guangzhou 510643GuangdongChina School of Energy and Environment City University of Hong KongHongkong 999077China Department of Physics South China University of TechnologyGuangzhou 510640GuangdongChina School of Chemistry and Chemical Engineering Guangzhou UniversityGuangzhou 510006GuangdongChina

Cocatalysts play important roles in improving the activity and stability of most *** is of great significance to develop economical,efficient and stable ***,using na2CoFe(Cn)6 complex as precursor,a novel noble-metal-free FeCo@ngC cocatalyst(nano-FeCo alloy.n-doped graphitized carbon) is fabricated by a simple pyrolysis *** with g-C3 n4, the optimal FeCo@ngC/g-C3n4 receives a boosted visible light driven photocatalytic H2 evolution rate of 42.2 μmol h-1, which is even higher than that of 1.0 wt% Pt modified g-C3n4 *** on the results of density functional theory(DFT) calculations and practical experiment measurements,such outstanding photocatalytic performance of FeCo@ngC/g-C3n4 is mainly attributed to two *** is the accelerated charge transfer behavior,induced by a photogene rated electrons secondary transfer performance on the surface of FeCo alloy *** other is related to the adjustment of H adsorption energy(approaching the standard hydrogen electrode potential) by the presence of external ngC thin *** factors play key roles in the H2 evolution *** outstanding performance highlights an enormous potential of developing noble-metal-free bimetallic nano-alloy as inexpensive and efficient cocatalysts for solar applications.

关键词： FeCo alloy.nanoparticles Cocatalyst n-doped graphitized carbon g-C3n4 Visible light Hydrogen evolution

Unravelling charge carrier dynamics in protonated g-C3n4 interfaced with carbon nanodots as co-catalysts toward enhanced photocatalytic CO2 reduction： A combined experimental and first-principles DFT study

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nano Research 2017年第5期10卷 1673-1696页

作者： Wee-Jun Ong Lutfi Kurnianditia Putri yoong-Chuen Tan Lling-Lling Tan neng Li y.n hau ng Xiaoming Wen Siang-Piao Chai Institute of Materials Research and Engineering (IMRE) Agency for Science Technology and Research (A'STAR) 2 Fusionopolis Way Innovis Singapore 138534 Singapore Multidisciplinary Platform of Advanced Engineering Chemical Engineering Discipline School of Engineering Monash University Jalan Lagoon Selatan Bandar Sunway 47500 Selangor Malaysia Chemical Engineering School of Engineering and Physical Sciences Heriot-Watt University Jalan Venna PS/2 Precinct 5 62200 Putrajaya Malaysia State Key Laboratory of Silicate Materials for Architectures Wuhan University of Technology 122 Luoshi Road Wuhan 430070 China Particles and Catalysis Research Group (PARTCAT) School of Chemical Engineering The University of New South Wales Sydney New South Wales 2052 Australia Australian Centre for Advanced Photovoltaics School of Photovoltaic and Renewable Energy Engineering The University of New South Wales Sydney New South Wales 2052 Australia

In this work, we demonstrated the successful construction of metal-free zero- dimensional/two-dimensional carbon nanodot （CnD）-hybridized protonatedg=C3n4 （pCn）（CnD/pCn） heterojunction photocatalysts b; means of electrostatic attraction. We experimentally found that CnDs with an average diameter of 4.4 nm were uniformly distributed on the surface of pCn using electron microscopy analysis. The CnD/pCn-3 sample with a CnD content of 3 wt.% showed thehighest catalytic activity in the CO2 photoreduction process under visible and simulated solar light. This process results in the evolution of CH4 and CO. Thetotal amounts of CH4 and CO generated by the CnD/pCn-3 photocatalyst after 10 h of visible-light activity were found to be 29.23 and 58.82 molgcatalyst-1, respectively. These values were 3.6 and 2.28 times higher, respectively, than thearn＊ounts generated when using pCn alone. The corresponding apparent quantum efficiency （AQE） was calculated to be 0.076%. Furthermore, the CnD/pCn-3 sample demonstrated high stability and durability after four consecutive photoreaction cycles, with no significant decrease in the catalytic activity.

关键词： protonated graphiticcarbon nitride carbon nanodots photocatalysis carbon dioxide reduction charge carrier dynamics density functional theory(DFT) calculations

A dual-electrolyte system for photoelectrochemical hydrogen generation using CuInS_2-In_2O_3-TiO_2 nanotube array thin film

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Science China Materials 2018年第6期61卷 895-904页

作者： Charlene ng Jung-Ho y.n Hui Ling Tan Hao Wu Rose Amal y.n hau ng Particles and Catalysis Research Group School of Chemical Engineering The University of New South Wales

The utilization of na2S/na2SO3 mixture as the electrolyte solution to stabilize sulfide anode in a photoelectrochemical cell for hydrogen evolution generally compromises the current-to-hydrogen efficiency（ηcurrent） of the system. Here, the employment of a dual-electrolyte system,that is, na2S/na2SO3 mixture and p H-neutral na2SO4 as the respective electrolyte solutions in the anode and cathode chambers of a water splitting cell is demonstrated to suppress the photocorrosion of CuInS2-In2O3-TiO2 nanotube（CISIn2O3-TnT） heterostructure, while simultaneously boosts theηcurrent. Although n-type CIS and In2O3 nanoparticles can be easily formed on TnT array via facile pulse-assisted electrodeposition method, conformal deposition of the nanoparticles homogeneously on the nanotubes wall with preservation of the TnT hollow structure is shown to be essential for achieving efficient charge generation and separation within the heterostructure. In comparison to na2S/na2SO3 solution as the sole electrolyte in both the anode and cathode chambers, introduction of dual electrolyte is shown to not only enhance the photostability of the CIS-In2O3-TnT anode, but also lead to near-unity ηcurrentas opposed to the merely 20% ηcurrentof the single-electrolyte system.

关键词： dual-electrolyte hydrogen generation photoelectrochemical TiO2 nanotubes CuInS2

n-doped graphitic carbon encapsulating cobalt nanoparticles derived from novel metal–organic frameworks for electrocatalytic oxygen evolution reaction

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中国化学快报:英文版 2023年第8期34卷 472-477页

作者： yuanmeng Tian Hao Wu Aamir Hanif y.nli niu y.ng y.n y.ngyi Gu Zuofeng Chen Qinfen Gu y.n hau ng Jin Shang Liangchun Li Mingxian Liu Shanghai Key Lab of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092China School of Energy and Environment City University of Hong KongHong Kong SAR 999077China City University of Hong Kong Shenzhen Research Institute Shenzhen 518000China Macao Institute of Materials Science and Engineering Faculty of Innovation EngineeringMacao University of Science and TechnologyMacao SAR 999078China Australian Synchrotron(AnSTO) Victoria 3168Australia

nitrogen-doped carbon catalysts with hierarchical porous structure are promising oxygen evolution reaction(OER)catalysts due to the faster mass transfer and better charge carry.ng ***,an exquisite high nitrogen-containing ligand was designed and readily synthesized from the low-cost biomolecule ***,three new MOFs(TJU-103,TJU-104 and TJU-105)were prepared using the Co(II)or Mn(II)ions as metal *** rationally controlling pyrolysis condition,in virtue of the high nitrogen content in well-defined periodic structure of the pristine MOFs,TJU-104–900 among the derived MOFs with hierarchical porous structure,i.e.,n-doped graphitic carbon encapsulating homogeneously distributed cobalt nanoparticles,could be conveniently *** to the synergistic effect of the hierarchical structure and well dispersed active components(i.e.,C=O,Co–nx,graphitic C and n,pyridinic n),it could exhibit an overpotential of 280 mV@10mA/cm^(2)on carbon cloth for OER *** work provides the inspiration for fabrication of nitrogen-doped carbon/metal electrocatalysts from cost-effective and abundant biomolecules,which is promising for practical OER application.

关键词： Metal-organic frameworks Oxygen evolution reaction High nitrogen content Cobalt nanoparticles Hierarchical structure

Energy transfer and luminescent properties of Tb^(3+)and Tb^(3+),yb^(3+)doped CngG phosphors

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Journal of Rare Earths 2022年第9期40卷 1445-1453,I0004页

作者： S.hau G.Stanciu D.Avram L.Gheorghe C.Gheorghe national Institute for Laser Plasma and Radiation PhysicsSolid State Quantum Electronics Laboratory409 Atomistilor StreetP.O.Box MG-36Magurele077125IlfovRomania

In this work,calcium niobium gallium garnet(Ca_(3)nb_(1.6875)Ga_(3.1875)O_(12)-CngG)ceramic samples singledoped with Tb^(3+)and co-doped with Tb^(3+)and yb^(3+)ions were sintered by the solid-state reaction *** structural characterization of the samples was carried out by X-ray diffraction *** optimal concentration of Tb^(3+)ions corresponding to the maximum luminescence in the green spectral range in CngG:x at%Tb(x=0.1,0.5,1,2,3,4,and 5)was determined to be 4 at%.The timeresolved luminescence of the^(5)D_(4)level(Tb^(3+))in the CngG:x at%Tb samples was analysed to explore the quenching mechanisms involved in the Tb^(3+)green ***-doped CngG:4 at%Tb,y at%yb(y=0.5,2,4,6,8,and 10)ceramics were prepared and *** is shown that CngG:4 at%Tb,y at%yb phosphors exhibit intense green luminescence under ultra-violet(UV),visible(VIS),and near-infrared(nIR)excitation,thus demonstrating the presence of simultaneous down-conversion(DC)and upconversion(UC)*** dependence of the UC luminescence intensity on the diode laser pumping power was measured and the results indicate a two-photon process based on cooperative energy transfer(CET).Under UV excitation,the lifetime of the^(5)D_(4)(Tb^(3+))level slowly increases with increase of yb^(3+)concentration,suggesting the energy transfer from yb^(3+)to Tb^(3+)ions,while under nIR excitation,the lifetime of the^(5)D_(4)(Tb^(3+))level decreases with increase of yb^(3+)ions concentration,indicating the presence of a strong energy transfer from Tb^(3+)to yb^(3+)*** highest energy transfer efficiency ofη_(ET)≈42%was determined for the CngG:4 at%Tb,10 at%yb *** obtained results indicate that CngG:(Tb^(3+),yb^(3+))could be efficient new yellowish-green-emitting phosphors.

关键词： Phosphors Tb^(3+)and Tb^(3+)-yb^(3+)luminescence properties Up-conversion Down-conversion Quantum cutting process Rare earths

Heterogeneous n-coordinated single-atom photocatalysts and electrocatalysts

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Chinese Journal of Catalysis 2022年第10期43卷 2453-2483页

作者： Rongchen Shen Lei Hao y.n hau ng Peng Zhang Arramel Arramel youji Li Xin Li Institute of Biomass Engineering Key Laboratory of Energy Plants Resource and Utilization Ministry of AgricultureSouth China Agricultural UniversityGuangzhou 511443GuangdongChina School of Energy and Environment City University of Hong KongHong KongChina Shenzhen Research Institute City University of Hong KongShenzhen Hi-Tech Industrial ParkShenzhen 518057GuangdongChina State Centre for International Cooperation on Designer Low-Carbon&Environmental Materials(CDLCEM) School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001HenanChina Department of Physics National University of SingaporeSingapore 117551Singapore nano Center Indonesia Jl.PUSPIPTEK South TangerangBanten 15314Indonesia College of Chemistry and Chemical Engineering Jishou UniversityJishou 416000HunanChina

Single-atom catalysts(SACs)have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined *** tailored coordination with nitrogen atom,the metal-nitrogen(M-n)-based SACs have demonstrated interesting physical,optical and electronic properties and have become intense in photocatalysis and electrocatalysis in the past *** substantial efforts in constructing various M–n-based SACs,the principles for modulating the intrinsic photocatalytic and electrocatalytic performance of their active sites and catalytic mechanism have not been sufficiently ***,the present review intends to shed some light on recent research made in study.ng the correlation between intrinsic electronic structure,catalytic mechanism,single-metal atom(SMA)confinement and their photocatalytic and electrocatalytic activities(conversion,selectivity,stability and etc).Based on the analysis of fundamentals of M–n-based SACs,theoretical calculations and experimental investigations,including synthetic methods and characterization techniques,are both included to provide an integral understanding of the underly.ng mechanisms behind improved coordination structure and observed ***,the challenges and perspectives for constructing highly active M–n based photocatalysis and electrocatalysis SACs are *** particular,extensive technical and mechanism aspects are thoroughly discussed,summarized and analyzed for promoting further advancement of M-n-based SACs in photocatalysis and electrocatalysis.

关键词： n-coordinated single-atom catalyst Photocatalysis Electrocatalysis Electronic structure Active site

A flexible capacitive photoreceptor for the biomimetic retina

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Light(Science & Applications) 2022年第1期11卷 38-49页

作者： Mani Teja Vijjapu Mohammed E.Fouda Agamyrat Agambayev Chun Hong Kang Chun-Ho Lin Boon S.Ooi Jr-hau He Ahmed M.Eltawil Khaled n.Salama Sensors lab Advanced Membranes and Porous Materials CenterComputerElectrical and Mathematical Science and Engineering DivisionKing Abdullah University of Science and Technology(KAUST)Thuwal 23955-6900Kingdom of Saudi Arabia Communication and Computing Systems Lab ComputerElectrical and Mathematical Science and Engineering DivisionKing Abdullah University of Science and Technology(KAUST)Thuwal 23955-6900Kingdom of Saudi Arabia Department of Electrical Engineering and Computer Science University of California-IrvineIrvineCA 92612USA Department of Electrical Computer and Energy EngineeringArizona State UniversityTempeAZUSA Computer Electrical and Mathematical Science and Engineering DivisionKing Abdullah University of Science and Technology(KAUST)Thuwal 23955-6900Kingdom of Saudi Arabia Department of Materials Science and Engineering City University of Hong KongHong Kong SARChina

neuromorphic vision sensors have been extremely beneficial in developing energy-efficient intelligent systems for robotics and privacy-preserving security *** is a dire need for devices to mimic the retina's photoreceptors that encode the light illumination into a sequence of spikes to develop such ***,we develop a hybrid perovskite-based flexible photoreceptor whose capacitance changes proportionally to the light intensity mimicking the retina's rod cells,paving the way for developing an efficient artificial retina *** proposed device constitutes a hybrid nanocomposite of perovskites(methyl-ammonium lead bromide)and the ferroelectric terpolymer(polyvinylidene fluoride trifluoroethylene-chlorofluoroethylene).A metal-insulator-metal type capacitor with the prepared composite exhibits the unique and photosensitive capacitive behavior at various light intensities in the visible light *** proposed photoreceptor mimics the spectral sensitivity curve of human photopic *** hybrid nanocomposite is stable in ambient air for 129 weeks,with no observable degradation of the composite due to the encapsulation of hybrid perovskites in the hydrophobic *** functionality of the proposed photoreceptor to recognize handwritten digits(MnIST)dataset using an unsupervised trained spiking neural network with 72.05%recognition accuracy is *** demonstration proves the potential of the proposed sensor for neuromorphic vision applications.

关键词： perovskite illumination preserving

Supramolecular Self-assembly of Amphiphilic Alkynylplatinum(II)2,6-Bis(n-alkylbenzimidazol-2′-yl)pyridine Complexes

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Chemical Research in Chinese Universities 2021年第5期37卷 1079-1084页

作者： Andy Shun-Hoi CHEUng Sammual yu-Lut LEUng Franky Ka-Wah hau Vivian Wing-Wah yAM Institute of Molecular Functional Materials and Department of Chemistry The University of Hong KongPokfulam RoadHong KongP.R.China

Alkynylplatinum(II)bzimpy complexes of trimethylammoniumbenzylethynyl ligand have been synthesized and *** with long alkyl chains have been found to exhibit interesting self-assembly properties in the acetonitrile *** amphiphilic nature of the complexes has led to the formation of nanorods,as revealed by electron microscopy *** increasing the polarity of the solvent media has given rise to the enhancement of low-energy emission.

关键词： solution. platinum alkyl