以泡沫镍(NF)为基底,通过一步水热法制备不同镍钴比的层状双氢氧化物(NiCoMo-LDH/NF)纳米催化剂,并借助X射线衍射和扫描电镜对催化剂的物相和形貌进行表征分析,研究催化剂元素组分调控对其电催化性能的影响。通过元素组分的调控,改变催化剂的显微结构,当Ni∶Co=1∶2(摩尔比,下同)时,Ni1Co2Mo-LDH/NF催化剂密集的纳米片结构,有利于活性位点的暴露和中间体吸脱附,以及电荷的快速传输,进而促使析氧反应的进行。电化学测试表明,在1mol/L KOH溶液中,电流密度达到10mA/cm2时,Ni∶Co=1∶2的纳米材料过电势仅为266mV,塔菲尔斜率为82.45mV/dec。此外,经12h的时间-电流稳定性测试后,材料的催化性能和形貌未有明显改变。可见,当Ni∶Co=1∶2时,材料表现出优异的催化活性和稳定性。
NiCoMo-LDH/NF nanocatalysts with different nickel-cobalt ratios were prepared by one-step hydrothermal method using nickel foam as the substrate.The phase and morphology of the catalysts were characterized by X-ray diffraction and scanning electron microscopy.The effect of catalyst element composition regulation on its electrocatalytic performance was investigated.The microstructure of the catalyst could be changed by adjusting the element composition.When molar ratio Ni∶Co=1∶2,the dense nanosheet structure of the Ni1Co2Mo-LDH/NF catalyst was beneficial to the exposure of active sites,the adsorption and desorption of intermediates and the rapid transfer of charge,which in turn promoted the oxygen evolution reaction.Electrochemical tests showed that in 1 mol/L KOH solution,when the current density reached 10mA·cm-2,the overpotential of the nanomaterial with molar ratio Ni∶Co=1∶2 was only 266mV,and the Tafel slope was 82.45mV·dec-1.In addition,the catalytic performance and morphology of the material did not change significantly after 12 h of time-current stability test.It was proven that when molar ratio Ni∶Co=1∶2,the material exhibited excellent catalytic activity and stability.
[1] Zou X,Zhang Y.Noble metal-free hydrogen evolution catalysts for water splitting[J].Chemical Society Reviews,2015,44(15):5148-5180.
[2] Ren X,Ge R,Zhang Y,et al.Cobalt-borate nanowire array as a high-performance catalyst for oxygen evolution reaction in near-neutral media[J].Journal of Materials Chemistry A,2017,5(16):7291-7294.
[3] Thenuwara A C,Shumlas S L,Attanayake N H,et al.Intercalation of cobalt into the interlayer of birnessite improves oxygen evolution catalysis[J].ACS Catalysis,2016,6(11):7739-7743.
[4] Esswein A J,Nocera D G.Hydrogen production by molecular photocatalysis[J].Chemical Reviews,2007,107(10):4022-4047.
[5] 汪广溪.氢能利用的发展现状及趋势[J].低碳世界,2017,29:295-296.
[6] 贺甜甜,邵若男,马腾飞,等.Al-Li-Ga-In-Sn合金水解产氢性能[J].河南科技大学学报(自然科学版),2020,41(3):1-5,117.
[7] Rusch L,Manz J,Hercinger M,et al.Nurse preceptor perceptions of nursing student progress toward readiness for practice[J].Nurse Educator,2019,44(1):34-37.
[8] He Q,Xie H,Rehman Z U,et al.Highly defective Fe-based oxyhydroxides from electrochemical reconstruction for efficient oxygen evolution catalysis[J].ACS Energy Letters,2018,3(4):861-868.
[9] Song F,Hu X.Ultrathin cobalt-manganese layered double hydroxide is anefficient oxygen evolution catalyst[J].Journal of the American Chemical Society,2014,136(47):16481-16484.
[10] Fan K,Chen H,Ji Y,et al.Nickel-vanadium monolayer double hydroxide forefficient electrochemical water oxidation[J].Nature Communications,2016,7:11981.
[11] Lu Z,Xu W,Zhu W,et al.Three-dimensional NiFe layered double hydroxide film for high-efficiency oxygen evolution reaction[J].Chemical Communications,2014,50(49):6479-6482.
[12] Li Z,Shao M,An H,et al.Fast electrosynthesis of Fe-containing layered double hydroxide arrays toward highly efficient electrocatalytic oxidation reactions[J].Chemical Science,2015,6(11):6624-6631.
[13] Luo J,Im J H,Mayer M T,et al.Water photolysis at 12.3% efficiency via perovskite photovoltaics and Earth-abundant catalysts[J].Science,2014,345(6204):1593-1596.
[14] Jiang J,Zhang A,Li L,et al.Nickel-cobalt layered double hydroxide nanosheets as high-performance electrocatalyst for oxygen evolution reaction[J].Journal of Power Sources,2015,278:445-451.
[15] Feng L,Du Y,Huang J,et al.NanoporousNiAl-LDH nanosheet arrays with optimized Ni active sites for efficient electrocatalytic alkaline water splitting[J].Sustainable Energy & Fuels,2020,4(6):2850-2858.
[16] Li P,Duan X,Kuang Y,et al.Tuning electronic structure of nife layered double hydroxides with vanadium doping toward high efficient electrocatalytic water oxidation[J].Advanced Energy Materials,2018,8(15):1703341.1-1703341.8.
[17] Long X,Xiao S,Wang Z,et al.Co intake mediated formation of ultrathin nanosheets of transition metal LDH—an advanced electrocatalyst for oxygen evolution reaction[J].Chemical Communications,2015,51(6):1120-1123.
[18] Wang J W,Wang Y F,Zhang J G,et al.Optimization of electrocatalytic properties of NiMoCo foam electrode for water electrolysis by post-treatment processing[J].Rare Metals,2015,34(11):802-807.
[19] Hu K,Wu M,Hinokuma S,et al.Boosting electrochemical water splitting via ternary NiMoCo hybrid nanowire arrays[J].Journal of Materials Chemistry A,2019,7(5):2156-2164.
[20] He W,Wei W,Wen B,et al.Lamellar NiMoCo@CuS enabling electrocatalytic activity and stability for hydrogen evolution[J].Chemical Communications,2019,55(71):10555-10558.
[21] Takeguchi T,Yamanaka T,Asakura K,et al.Evidence of nonelectrochemical shift reaction on a CO-tolerant high-entropy state Pt-Ru anode catalyst for reliable and efficient residential fuel cell systems[J].Journal of the American Chemical Society,2012,134(35):14508-14512.
[22] 李春,田朋,庞洪昌,等.钨掺杂的铁镍基层状氢氧化物用于电催化析氧和析氢反应[J].无机化学学报,2020,36(8):1492-1498.
[23] Liu H,Zhao D,Liu Y,et al.NiMoCo layered double hydroxides for electrocatalyst and supercapacitor electrode[J].Science China Materials,2021,64(3):581-591.
[24] Li X,Lin S Y,Zhang M,et al.Construction of hierarchical Ni(OH)2@CoMoO4 nanoflake composite for high-performance supercapacitors[J].Nano,2016,11(5):1650050.
[25] 王志强,刘卫红,耿凤霞.过渡金属层状双氢氧化物电催化剂研究进展[J].中国材料进展,2017,36(9):659-666.
[26] Watzele S A.Methodological aspects of in-depth electrochemical characterization of metal and metal oxide electrocatalysts[D].München:Technische Universität München,2020.
[27] Pintado S,Goberna-Ferrón S,Escudero-Adán E C,et al.Fast and persistent electrocatalytic water oxidation by Co-Fe prussian blue coordination polymers[J].Journal of the American Chemical Society,2013,135(36):13270-13273.
[28] Ge R,Ren X,Ji X,et al.Benzoate anion-intercalated layered cobalt hydroxide nanoarray:an efficient electrocatalyst for the oxygen evolution reaction[J].ChemSusChem,2017,10(20):4004-4008.
基金资助
国家自然科学基金资助项目(51901070);河南科技大学大学生研究训练计划项目(2020042)
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