Cobalt atomic clusters-polytungsten metal-oxygen clusters-carbon black composites (CoClusters-SiW12-CB abbreviated as Co-SiW12-CB) were prepared by impregnation method and annealed in air at 160℃.The materials were characterized and analysed by X-ray diffraction analysis (XRD),transmission electron microscopy (TEM),high-angle annular dark-field scanning projection electron microscopy (HADDF-STEM),X-ray photoelectron spectroscopy (XPS) and X-ray energy spectrometry (EDS),and BET tests were performed to characterize and analyze the materials and test their hydrogen precipitation properties.The results showed that the Co atomic clusters could be stably anchored on the surface thanks to the metal-carrier interaction.The required overpotential for the hydrogen precipitation reaction was 423mV with a Tafel slope of 119mV/dec in 1.0mol/L KOH alkaline electrolyte when the current density was 10mA/cm2.In addition,the catalytic materials were more stable and had better electrochemical hydrogen precipitation performance in alkaline electrolyte.
[1] Zhou F,Zhou Y,Liu G,et al.Recent advances in nanostructured electrocatalysts for hydrogen evolution reaction[J].Rare Metals,2021,40(12):3375-3405.
[2] Seyitoglu S S,Dincer I,Kilicarslan A.Energy and exergy analyses of hydrogen production by coal gasification[J].International Journal of Hydrogen Energy,2016,42(4):2592-600.
[3] Seh Z W,Kibsgaard J,Dickens C F,et al.Combining theory and experiment in electrocatalysis:insights into materials design[J].Science,2017,355(6321):1-12.
[4] 葛靖暄,胡钧,朱盈婷,等.多酸在电催化析氢反应中的应用研究进展[J].物理化学学报,2020,36(1):83-102.
[5] Lu K,Liu Y Z,Lin F,et al.LixNiO/Ni heterostructure with strong basic lattice oxygen enables electrocatalytic hydrogen evolution with Pt-like activity[J].Journal of the American Chemical Society,2020,142(29):12613-12619.
[6] Li M F,Duanmu K N,Wan C Z,et al.Single-atom tailoring of platinum nanocatalysts for high-performance multifunctional electrocatalysis[J].Nature Catalysis,2019,2(6):495-503.
[7] Talib S H,Lu Z,Yu X,et al.Theoretical inspection of M1/PMA single-atom electrocatalyst:ultra-high performance for water splitting (HER/OER) and oxygen reduction reactions (OER)[J].ACS Catalysis,2021,11(14):8929-8941.
[8] Wang C,Chen F,Wang Q,et al.Defect-stabilized platinum single atoms and clusters in bilayer nitrogen-doped porous carbon nanocages for synergistic catalysis of basic hydrogen evolution[J].Carbon,2023,201(11):278-284.
[9] Liu X,Huang D,Lai C,et al.Single cobalt atom anchored on carbon nitride with cobalt nitrogen/oxygen active sites for efficient fenton-like catalysis[J].Journal of Colloid and Interface Science,2023,629:417-427.
[10] Guo D,Huang Z,Liu Y,et al.Incorporation of single-atom copper into nitrogen-doped graphene for acetaminophen electrocatalytic degradation[J].Applied Surface Science,2022,604(4):154561.
[11] Ou H,Wang D,Li Y.How to select effective electrocatalysts:nano or single atom？[J].Nano Select,2021,2(3):492-511.
[12] Lv Y,Wu X Y,Lin H,et al.A novel carbon support:few-layered graphdiyne-decorated carbon nanotubes capture metal clusters as effective metal-supported catalysts[J].Small,2021,17(12):20064421-200644210.
[13] Zhang B,Sun G,Ding S,et al.Atomically dispersed Pt1-polyoxometalate catalysts:how does metal-support interaction affect stability and hydrogenation activity？[J].Journal of the American Chemical Society,2019,141(20):8185-8197.
[14] Zhang S,Liu R,Streb C,et al.Design and synthesis of novel polyoxometalate-based binary and ternary nanohybrids for energy conversion and storage[J].Polyoxometalates,2023,2(1):9140037.
[15] Bai X,Huang X,Wen L,et al.A new strategy for the selective oxidation of alcohols catalyzed by a polyoxometalate-based hybrid surfactant in biphasic systems[J].Chemical Communications,2019,55(25):3598-3601.
[16] Li X X,Zhao D,Zheng S T.Recent advances in POM-organic frameworks and POM-organic polyhedra[J].Coordination Chemistry Reviews,2019,397(10):220-240.
[17] Zhang B,Asakura H,Zhang J,et al.Stabilizing a platinum single-atom catalyst on supported phosphomolybdic acid without compromising hydrogenation activity[J].Angewandte Chemie-International Edition,2016,55(29):8319-8323.
[18] Liu R J,Streb C.Polyoxometalate-single atom catalysts (POM-SACs) in energy research and catalysis[J].Advanced Energy Materials,2021,11(25):21011201-210112013.
[19] Liu Q,Wang X.Polyoxometalate clusters:sub-nanometer building blocks for construction of advanced materials[J].Matter,2020,2(4):816-841.
[20] Zhang T R,Weng S T,Wang X F,et al.Platinum atomic clusters embedded in polyoxometalates-carbon black as an efficient and durable catalyst for hydrogen evolution reaction[J].Journal of Colloid and Interface Science,2022,624:704-712.
[21] Zang Y,Niu S,Wu Y,et al.Tuning orbital orientation endows molybdenum disulfide with exceptional alkaline hydrogen evolution capability[J].Nature Communications,2019,10(1):1-8.
[22] Xiao J,Lv Q,Zhang Y,et al.One-step synthesis of nickel phosphide nanowire array supported on nickel foam with enhanced electrocatalytic water splitting performance[J].RSC Advances,2016,6(109):107859-107864.
[23] Zhou D,Han B H.Graphene-based nanoporous materials assembled by mediation of polyoxometalate nanoparticles[J].Advanced Functional Materials,2010,20(16):2717-2722.
[24] 陈理,黄伟国,刘孝伟,等.不同碳材料对铅炭负极的性能影响[J].储能科学与技术,2018,7(6):1248-1252.
[25] 于霞,王垚,郗瑜,等.酞菁钴功能化钒取代多金属氧酸盐催化剂的合成及氧化脱硫性能[J].东北师大学报(自然科学版),2024,56(1):101-106.
[26] Gao J J,Hu Y X,Wang Y,et al.MOF Structure engineering to synthesize Co-N-C catalyst with richer rccessible active sites for enhanced oxygen reduction[J].Small,2021,17(49):21046841-21046849.
[27] Wang Q,Huang X,Zhao Z L,et al.Ultrahigh-loading of Ir single atoms on NiO matrix to dramatically enhance oxygen evolution reaction[J].Journal of the American Chemical Society,2020,142(16):7425-7433.
[28] Nemiwal M,Zhang T C,Kumar D.Graphene-based electrocatalysts:hydrogen evolution reactions and overall water splitting[J].International Journal of Hydrogen Energy,2021,46(41):21401-21418.
[29] Cai C,Wang M,Han S,et al.Ultrahigh oxygen evolution reaction activity achieved using Ir single atoms on amorphous CoOx nanosheets[J].ACS Catalysis,2021,11(1):123-130.
[30] Lu X,Zhao C.Electrodeposition of hierarchically structured three-dimensional nickel-iron electrodes for efficient oxygen evolution at high current densities[J].Nature Communications,2015,6(1):1-7.
基金资助
国家自然科学基金(21862005)
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