高等学校化学学报 ›› 2022, Vol. 43 ›› Issue (5): 20220065.doi: 10.7503/cjcu20220065
收稿日期:
2022-01-26
出版日期:
2022-05-10
发布日期:
2022-03-03
通讯作者:
李煜璟
E-mail:yjli@bit.edu.cn
基金资助:
CHEN Changli1, MI Wanliang2, LI Yujing1()
Received:
2022-01-26
Online:
2022-05-10
Published:
2022-03-03
Contact:
LI Yujing
E-mail:yjli@bit.edu.cn
Supported by:
摘要:
单原子催化剂(SACs)是一类仅含有孤立的单个金属原子作为催化活性中心的催化材料. 由于其具有100%的原子利用率、 独特的化学结构及优异的催化活性等优点, 近年来在电化学催化和电能转换设备领域备受关注. 本文综合评述了单原子催化材料的设计理念、 合成方法和表征方法, 同时对其在氢电化学循环 (电解水制氢和氢燃料电池领域)的实际应用进行了系统介绍, 并对单原子催化材料的研究和应用前景进行了展望.
中图分类号:
TrendMD:
陈长利, 米万良, 李煜璟. 单原子催化材料在电化学氢循环应用中的研究进展. 高等学校化学学报, 2022, 43(5): 20220065.
CHEN Changli, MI Wanliang, LI Yujing. Research Progress of Single Atom Catalysts in Electrochemical Hydrogen Cycling. Chem. J. Chinese Universities, 2022, 43(5): 20220065.
Fig.1 Numbers of published literatures from 2011 to 2021 by the keyword “single atom catalysts” in all database of web of scienceThe inset pie diagram reflects the percentages of the literatures from by the keyword combination of “single atom catalysts” and “ORR/Fuel cell” or “HER” or “OER” or “Water splitting”, respectively.
Fig.2 Preparation and morphology characterization of Fe?SAs/NSC(A)[26], schematic illustration of the preparation of Pt@DG(B)[28], schematic illustration of the synthetic process for W0.25Mo0.75P/PNC(C)[30] and scheme showing host?guest strategy for the fabrication of single?atomic?site catalysts(D)[31](A) Copyright 2019, American Chemical Society; (B) Copyright 2022, American Chemical Society; (C) Copyright 2021, American Chemical Society; (D) Copyright 2019, American Chemical Society.
Fig.4 Seamlessly conductive electrode structure as a highly efficient electrocatalyst for the HER(A), linear sweep voltammetry(LSV) curves of PtSA?Co(OH)2@Ag NW, Co(OH)2@Ag NW, Co@Ag NW, Ag NWs, the Pt sheet and Pt/C(20%, mass fraction)(B), calculated PDOS of d orbitals of bulk Pt, PtSA?Co(OH)2 and Co(OH)2(C), calculated adsorption energies of H and H2O on the surface of Co(OH)2, PtSA?Co(OH)2 and bulk Pt(D)[60]Copyright 2020, the Royal Society of Chemistry.
Fig.5 OER current curves of Ni?O?G SACs, NiO, B Ni?O?G, Ni?N?G SACs, O?G, and RuO2 in 1 mol/L KOH(A), chronoamperometric curve of Ni?O?G SACs obtained at constant overpotential of 400 mV in 1 mol/L KOH(B), optimized geometric model of Ni sites in Ni?O?G SACs structure(C), the corresponding map of the DFT ESP surfaces of Ni?O?G SACs structure(D), schemeric of oxygen production pathways on the Ni site within Ni?O?G SACs geometry(E), the free?energy diagrams of OER pathways and OER theoretical overpotential of the Ni?O?G SACs structure(red), Ni?N?G SACs(pink), and NiO nanoparticles(blue)(F)[69]Inset of (B) is the corresponding HAADF?STEM image of Ni?O?G SACs after 50 h durability test, the single Ni atoms show bright dots marked with red circles. (D) Blue color indicates positive charges, and red color indicates negative charge. Copyright 2020, Wiley?VCH.
Fig.6 Illustration of the working mechanism of the prepared electrodes(A), the polarization curves of overall water splitting by the Ir1@Co/NC catalyst(B), the free?energy diagrams for the HER at pH=14 on IrNC3, IrC4, Ir1@Co(Co), and Ir1@Co(Ir)(C), the reaction free energies for the OER at pH=14 of the intermediates on Ir1@CoO(Co)(D) and Ir1@CoO(Ir)(E)[10]Inset of (B) is image of a two?electrode system producing bubbles of H2 and O2 at an applied potential of 1.4 V(vs. RHE). Copyright 2019, Wiley?VCH.
Fig.8 Plan view of presumed porphyrin?like CoN4C10 sites in the micropores(A), ORR polarization plots for different Co(mIm)?NC catalysts in 0.1?mol/L HClO4 under O2 saturation(B), fuel cell performance of Co(mIm)?NC(1.0) measured under 1.0×105 Pa H2/O2 and H2/air(C), durability tests of the Co(mIm)?NC(1.0) and Fe(mIm)?NC(1.0) catalysts in MEA in 1×105 Pa H2/air at a constant cell voltage of 0.7?V for 100?h(D), in situ CO2 emission test from the fuel cell cathode with the Co(mIm)?NC(1.0) catalyst(E), normalized current density at a voltage of 0.85?V after voltage?step cycling(0.4?V for 55?min and 0.85?V for 5?min) for 50?h(cycles) measured under 1.0×105 Pa H2/O2(F), ICP?OES and RRDE(E1/2) results of the metal leaching experiments(G), atomistic structures of simulation models of porphyrin?like MN4C12(M?=?Fe or Co) active sites and their corresponding O2 adsorption configurations on the M site(H), predicted thermochemical constants of losing an M atom from the porphyrin?like MN4C12(M?=?Fe or Co) sites(I)[94](H) C: grey, N: blue, M: purple, O: red, H: white. Copyright 2020, Springer Nature.
Fig.9 Current density?voltage(solid) and current density?power density(dashed) curves for a H2/O2 AEMFC with a cathode with 1?mg/cm2 Fe?N?C, an anode with 0.6?mg/cm2 PtRu(A), voltage, HFR and current versus time curves recorded at a constant current density of 600?mA/cm2(B), comparison of the specific peak power(W/mgPGM loading) with H2/O2 for different AEMFCs, both state?of?the?art PGM?type cells and those employing PGM?free electrocatalysts(C)[97]Copyright 2021, Springer Nature.
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