高等学校化学学报 ›› 2022, Vol. 43 ›› Issue (5): 20220051.doi: 10.7503/cjcu20220051
收稿日期:
2022-01-23
出版日期:
2022-05-10
发布日期:
2022-03-03
通讯作者:
费慧龙
E-mail:hlfei@hnu.edu.cn
基金资助:
WU Jun, HE Guanchao, FEI Huilong()
Received:
2022-01-23
Online:
2022-05-10
Published:
2022-03-03
Contact:
FEI Huilong
E-mail:hlfei@hnu.edu.cn
Supported by:
摘要:
单原子催化剂的催化活性高, 稳定性强, 原子利用率高, 在能源电催化领域已被广泛研究. 然而, 粉末状(颗粒状)单原子催化材料存在工作电极制备过程复杂、 黏结剂添加降低导电性且占据催化材料的体积、 活性位点易被包埋等问题, 在作为电极材料催化能源转化过程时, 载量通常小于1 mg/cm2, 反应电流密度不高于100 mA/cm2. 与单原子催化剂相比, 自支撑单原子膜电极不仅具有单原子催化剂的诸多优势, 同时展现出整体式电极的特点, 例如无需添加黏结剂、 导电性好、 单原子活性位点暴露率高、 形貌与孔结构可调控等, 在大电流电催化反应、 高能量高功率密度电池等领域拥有应用前景. 本文综合评述了面向能源电催化应用的自支撑单原子膜电极的研究进展, 讨论了自支撑单原子膜电极的优势, 总结了自支撑单原子膜电极的合成方法, 包括自支撑基底上原位制备法、 静电纺丝法、 自组装法、 化学气相沉积与固相扩散法等, 介绍了其在析氢反应、 析氧反应、 电化学制过氧化氢反应、 锌空电池、 二氧化碳还原反应及锂硫电池中的应用, 并对该类电极的发展方向进行了展望.
中图分类号:
TrendMD:
吴俊, 何观朝, 费慧龙. 自支撑单原子膜电极在能源电催化中的应用. 高等学校化学学报, 2022, 43(5): 20220051.
WU Jun, HE Guanchao, FEI Huilong. Self-supported Film Electrodes Decorated with Single Atoms for Energy Electrocatalysis. Chem. J. Chinese Universities, 2022, 43(5): 20220051.
Fig.1 Schematic illustrations for the synthesis of SS?CoSAC(A)[12], NiRu?LMH ultrathin nanoribbons(R?NiRu) and nanosheets(S?NiRu)(B)[20], and np?Ir/NiFeO(C)[23](A) Copyright 2019, Wiley-VCH; (B) Copyright 2021, Wiley-VCH; (C) Open access.
Fig.4 Scheme for the synthesis of H?CPs(A)[15], Ni@NCNTs?CNF catalysts(B)[35] and the SAFe?SWCNT film(C)[36](A) Copyright 2018, Elsevier; (B) Copyright 2020, Elsevier; (C) Copyright 2021, Elsevier.
Fig.5 Schematic illustration of the fabrication procedure(A), SEM image(B), HAADF?STEM images and the corresponding EDS mapping images(C), Aberration?corrected HAADF?STEM images with the bright points representing Fe atoms(D) of the SAC?FeN?WPC[41]Copyright 2021, American Chemical Society.
Fig.6 HER polarization curves of different catalysts, acquired with 5 mV/s in N2?saturated 1.0 mol/L PBS(A), SEM images of PtSA?NT?NF(B)[43], linear sweep voltammetry(LSV) curves in 0.5 mol/L H2SO4 at the scan rate of 5 mV/s for different catalysts along with Pt foil and Pt/C as reference point(C), stability of Co?NC?AF evaluated by the galvanostatic technique(D) and snapshot of H2 bubbles detaching from Co?NC?AF(E) at the current density of 100 mA/cm2[10](A, B) Copyright 2017, Wiley-VCH; (C—E) Copyright 2021, Wiley-VCH.
Fig.7 OER polarization curves of np?NiFeO, np?Ir/NiFeO and IrO2(A), corresponding Tafel plots(B) of the presented data in (A), stability of np?Ir/NiFeO evaluated by the current density versus time(i?t) curves at 1.43 V versus RHE with inset showing the CV curves of np?Ir/NiFeO before and after the acceleration durability test for 3000 cycles(C), operando XANES spectra of np?Ir/NiFeO recorded at Ir L3?edge under different applied voltages from OCV to 1.55 V versus RHE in 1.0 mol/L KOH(D), correspon?ding first?shell(Ir—O) fitting of FT?EXAFS spectra for np?Ir/NiFeO(E), the fitted oxidation states from the white line intensity analysis, the variation of Ir—O bond and the FT?EXAFS curve?fitting analysis(F), calculated free energy diagram of the OER(G), the Gibbs free energy of the rate?determining step for different sites(H), scheme for the shrinkage of the Ni(Fe)—O bonds determined by the operando XAS analysis of np?Ir/NiFeO(I)[22](G) The blue box step is the rate?determining step. Open access.
Fig.9 Field emission scanning electron microscope(FESEM) image of Co SA@NCF/CNF film(A), ORR LSV curves of Co SA@NCF/CNF, Co NP@NCF/CNF, and Pt/C in 0.1 mol/L KOH electrolyte(B), OER LSV curves of Co SA@NCF/CNF, Co NP@NCF/CNF, Ir/C, and Pt/C in 1.0 mol/L KOH electrolyte(C), the voltage?capacity curves of the prepared ZABs(D), discharge curves of the prepared ZABs at different current densities and testing conditions(E)[28], galvanostatic discharge/charge cycling curves and the corresponding power density of an SAC?FeN?WPC plate?based quasi?solid?state battery(F)[41](A—E) Copyright 2019, Wiley-VCH; (F) Copyright 2021, American Chemical Society.
Fig.10 Water contact angles, underwater gas bubble contact angles and schematic illustration of H?CPs(A) and Ni SAs/CFPs(B)[15], partial current densities of NiSA/PCFM at various cathode potentials in GDE cell and H?type cell(C), stability tests of NiSA/PCFM in GDE cell at -1.0 VRHE(D), partial current densities for different catalysts at various cathode potentials in H?type cell(E) and stability tests of P?NiSA/PCFM in H?type cell at -1.0 VRHE(F)[30](A, B) Copyright 2019, Elsevier; (C—F) open access.
Fig.11 Comparison of the areal capacity of the SATi@CF/S cathode and commercial Li?ion batteries at diffe?rent rates(A), rate performance of different cathodes(B), SEM images of the final Li2S deposit on CF and SATi@CF surfaces(C)[65], schematic configuration of a conventional Li?S full battery and Co?PCNF dual?functional fibrous skeleton enabled Li?S full battery(D), areal capacity of S/Co?PCNF||Co?PCNF@Li full batteries obtained at 0.1C with different sulfur loadings(E)[61](A—C) Copyright 2021, Wiley-VCH; (D, E) Copyright 2021, American Chemical Society.
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