高等学校化学学报 ›› 2023, Vol. 44 ›› Issue (1): 20220666.doi: 10.7503/cjcu20220666
收稿日期:
2022-10-10
出版日期:
2023-01-10
发布日期:
2022-11-15
通讯作者:
赖小勇
E-mail:xylai@nxu.edu.cn
基金资助:
YANG Qingfeng, LYU Liang, LAI Xiaoyong()
Received:
2022-10-10
Online:
2023-01-10
Published:
2022-11-15
Contact:
LAI Xiaoyong
E-mail:xylai@nxu.edu.cn
Supported by:
摘要:
水分裂、 金属-空气电池和燃料电池等能源转换技术对解决未来的能源危机和环境问题至关重要. 氧还原反应(ORR)、 氧析出反应(OER)和氢析出反应(HER)作为其核心反应, 存在反应动力学速率较慢的问题, 因此, 开发研制高效的非贵金属电催化剂具有重要意义. 金属有机骨架(MOFs)材料因具有高度可调的组成和多孔晶体结构, 在不同的应用领域引起了越来越多的关注. 中空MOFs纳米材料具有MOFs材料高度可调的组成和结构优势, 又具有中空结构纳米材料的优点(如更快的物质传输、 更丰富的孔隙率、 灵活多变的活性组分、 更多的暴露活性位点及对苛刻条件的更好相容性等), 在电催化领域显现出巨大的应用潜力. 本文对近几年来基于中空结构MOFs材料的制备及在电催化方面应用的研究进展进行了综合评述, 并对该领域面临的挑战和发展前景进行了总结和展望.
中图分类号:
TrendMD:
杨庆凤, 吕良, 赖小勇. 中空MOFs材料制备及电催化应用的研究进展. 高等学校化学学报, 2023, 44(1): 20220666.
YANG Qingfeng, LYU Liang, LAI Xiaoyong. Progress on Preparation and Electrocatalytic Application of Hollow MOFs. Chem. J. Chinese Universities, 2023, 44(1): 20220666.
Fig.1 Scheme of preparation of polystyrene@ZIF⁃8 core⁃shell and hollow ZIF⁃8 microspheres from carboxylate⁃terminated polystyrene spheres[63]Copyright 2012, the Royal Society of Chemistry.
Fig.4 Illustration of the procedure for synthesizing hollow MOF tubes(A) and the protein⁃induced hollow MOF⁃based composite spheres(B)[78]Copyright 2019, Wiley-VCH.
Fig.5 Spray⁃drying synthesis of spherical hollow HKUST⁃1 superstructures[80](A) Schematic showing the spray-drying process used to synthesize HKUST-1 superstructures; (B) proposed spherical superstructure formation process(emphasized by purple arrows), which implies the crystallization of nano MOF crystals; (C) photograph of the spray-dryer after its use in synthesizing large amounts of blue HKUST-1 superstructures; (D—F) representative FESEM images showing a general view of the spherical HKUST-1 superstructures[scale bars: 5 mm(D), 500 nm(E,F), 200 nm(F, inset)].Copyright 2013, Springer Nature.
Fig.7 Deposition of a MOF layer on a support in a homogeneous synthesis mixture(A) and interfacial preparation of a MOF layer using a biphasic synthesis mixture consisting of an aqueous metal⁃ion⁃containing solution and an organic ligand solution(B)[84]Copyright 2011, Springer Nature.
Fig.8 Schematic illustrating the synthesis of MIL⁃88A MOF hollow architectures using the microfluidic approach[85]Copyright 2015, American Chemical Society.
Fig.13 Schematic process of hollow MOFs etched by HNO3 and ROS from inside to outside or from outside to interior[94]Copyright 2019, American Chemical Society.
Year | Composition | Morphology | Size/nm | Specific area/(m2·g-1) | Preparation characteristics | Ref. |
---|---|---|---|---|---|---|
2011 | [Cu3(BTC)2] | Capsules | 375000 | 620 | Liquid⁃liquid interface | [ |
2012 | ZIF⁃8 | Microspheres | 970 | — | Hard⁃templating | [ |
2012 | Pd@ZIF⁃8 | Yolk⁃shell | 430 | 1643 | Hard⁃templating | [ |
2013 | HKUST⁃1 | Discrete octahedral | 75±28 | 1260 | Gas⁃liquid interface | [ |
2014 | Zn/Ni⁃MOFs⁃2 | Nanocubes | 300—500 | 433 | Solid⁃liquid interface | [ |
2015 | ZIF⁃8 | Nanospheres | 250 | — | Soft⁃templating | [ |
2015 | MIL⁃88A | Capsules | 440000 | — | Liquid⁃liquid interface | [ |
2016 | ZIF⁃67 | Prismatic | 480 | 28.1 | Solid⁃liquid interface | [ |
2017 | Cr⁃MOF(MIL⁃101) | Yolk⁃shell | 350 | 2847 | Selective etching | [ |
2018 | HNTM⁃Ir/Pt | Nanotubes | 1000 | 844 | Coordination modulation | [ |
2019 | ZIF⁃8 | Nanospheres | 300 | 1012 | Soft⁃templating | [ |
2019 | UiO⁃66(OH)2 | Octahedral⁃shaped particles | 400 | — | Selective etching | [ |
2019 | Co3S4/EC⁃MOF | Echinops⁃like | 500 | 110.1 | Hard⁃templating | [ |
2020 | Fe@NiCo⁃MOF HNSs | Nanospheres | 840 | 257 | Solvothermal | [ |
2020 | Ni/Co⁃MOFs | Yolk⁃shell | 3000 | 68 | Ion induction | [ |
2020 | MOF⁃5@ZIF⁃8 | Yolk⁃shell | 800 | — | Coordination modulation | [ |
2021 | Ru@NiCo⁃MOF HPNs | Porous nanospheres | 855 | — | Hydrothermal | [ |
2021 | CoCu⁃MOF NBs | Nanobox | 100 | 307 | Coordination modulation method | [ |
2021 | NiFe⁃MOFs | Nano bricks | 1600 | 17.22 | Solvothermal | [ |
2021 | H⁃PMOF | Mesoporous spherical shell | 90 | 120 | Hard⁃templating | [ |
2022 | PdAg@ZIF⁃8 | Yolk⁃shell | 350—450 | 1035 | Hard⁃templating | [ |
2022 | ZIF⁃8⁃HS | Nanospheres | 1000 | 1195 | Soft⁃templating | [ |
2022 | HM⁃MIL | Irregular octahedral | 220 | 941.47 | Selective etching | [ |
Table 1 Summary of different types of hollow MOFs
Year | Composition | Morphology | Size/nm | Specific area/(m2·g-1) | Preparation characteristics | Ref. |
---|---|---|---|---|---|---|
2011 | [Cu3(BTC)2] | Capsules | 375000 | 620 | Liquid⁃liquid interface | [ |
2012 | ZIF⁃8 | Microspheres | 970 | — | Hard⁃templating | [ |
2012 | Pd@ZIF⁃8 | Yolk⁃shell | 430 | 1643 | Hard⁃templating | [ |
2013 | HKUST⁃1 | Discrete octahedral | 75±28 | 1260 | Gas⁃liquid interface | [ |
2014 | Zn/Ni⁃MOFs⁃2 | Nanocubes | 300—500 | 433 | Solid⁃liquid interface | [ |
2015 | ZIF⁃8 | Nanospheres | 250 | — | Soft⁃templating | [ |
2015 | MIL⁃88A | Capsules | 440000 | — | Liquid⁃liquid interface | [ |
2016 | ZIF⁃67 | Prismatic | 480 | 28.1 | Solid⁃liquid interface | [ |
2017 | Cr⁃MOF(MIL⁃101) | Yolk⁃shell | 350 | 2847 | Selective etching | [ |
2018 | HNTM⁃Ir/Pt | Nanotubes | 1000 | 844 | Coordination modulation | [ |
2019 | ZIF⁃8 | Nanospheres | 300 | 1012 | Soft⁃templating | [ |
2019 | UiO⁃66(OH)2 | Octahedral⁃shaped particles | 400 | — | Selective etching | [ |
2019 | Co3S4/EC⁃MOF | Echinops⁃like | 500 | 110.1 | Hard⁃templating | [ |
2020 | Fe@NiCo⁃MOF HNSs | Nanospheres | 840 | 257 | Solvothermal | [ |
2020 | Ni/Co⁃MOFs | Yolk⁃shell | 3000 | 68 | Ion induction | [ |
2020 | MOF⁃5@ZIF⁃8 | Yolk⁃shell | 800 | — | Coordination modulation | [ |
2021 | Ru@NiCo⁃MOF HPNs | Porous nanospheres | 855 | — | Hydrothermal | [ |
2021 | CoCu⁃MOF NBs | Nanobox | 100 | 307 | Coordination modulation method | [ |
2021 | NiFe⁃MOFs | Nano bricks | 1600 | 17.22 | Solvothermal | [ |
2021 | H⁃PMOF | Mesoporous spherical shell | 90 | 120 | Hard⁃templating | [ |
2022 | PdAg@ZIF⁃8 | Yolk⁃shell | 350—450 | 1035 | Hard⁃templating | [ |
2022 | ZIF⁃8⁃HS | Nanospheres | 1000 | 1195 | Soft⁃templating | [ |
2022 | HM⁃MIL | Irregular octahedral | 220 | 941.47 | Selective etching | [ |
Fig.14 LSV curves of NiCo⁃MOF HNSs, Fe@NiCo⁃MOF HNSs and Ir/C in 1 mol/L KOH aqueous solution(A), the corresponding overpotentials and current densities of different electrocatalysts at 10 mA/cm2 and 1.53 V(vs. RHE), respectively(B), corresponding Tafel slopes(C) and LSV curves for Fe@NiCo⁃MOF HNSs before and after 1000 cycles of CV scans(D)[97]Copyright 2020, the Royal Society of Chemistry.
Fig.15 LSV curves of Ru@NiCo⁃MOF⁃2, Ru@NiCo⁃MOF⁃4 and Ru@NiCo⁃MOF⁃6(A), the required overpotentials of Ru@NiCo⁃MOF⁃2, Ru@NiCo⁃MOF⁃4, and Ru@NiCo⁃MOF⁃6 at current densities of 10 and 30 mA/cm2(B), capacitive current density(C) and Tafel plots(D) of Ru@NiCo⁃MOF⁃2, Ru@NiCo⁃MOF⁃4 and Ru@NiCo⁃MOF⁃6[98]Copyright 2021, American Chemical Society.
Fig.16 LSV plots(A) and the overpotential(B) at 10 mA/cm2 for RuO2, Cu⁃MOF NPs, Co⁃MOF NBs and CoCu⁃MOF NBs, the corresponding Tafel slopes(C) and TOF values(D) under an overpotential of 300 mV for RuO2, Cu⁃MOF NPs, Co⁃MOF NBs and CoCu⁃MOF NBs, the capacitive current density(ΔJ/2) at 1.05 V(vs. RHE) against the scan rate for Cu⁃MOF NPs, Co⁃MOF NBs and CoCu⁃MOF NBs(E) and I⁃t curves for CoCu⁃MOF NBs and RuO2(F)[99]Copyright 2021, Wiley-VCH.
Fig.17 LSV curves(A), corresponding Tafel plots(B) and overpotentials(C) at a current density of 10 mA/cm2 of NiFe⁃MOFs/NF nanobrick arrays and RuO2/NF in 1 mol/L KOH aqueous solution, chronopotentiometry curves of NiFe⁃MOFs/NF nanobrick arrays for 24 h at high current densities of 50 and 100 mA/cm2(D)[100]Copyright 2022, Springer.
Fig.18 HER(A) and OER(B) curves obtained with MOFs catalysts and precious metal⁃based benchmark catalysts, chronopotentiometry(E⁃t) plot obtained with NCF⁃MOF at a fixed applied current density of -20 mA/cm2 for HER and 20 mA/cm2 for OER(C), OER polarization curves of NCF⁃MOF and Ir/C before and after 1000 CV cycles(D)[101](C)The inset shows the changes in the overpotentials during chronopotentiometric HER and OER tests, and the corresponding potential retentions.Copyright 2018, Wiley-VCH.
Fig.19 ORR LSV profiles of the different catalysts(conditions: 0.1 mol/L KOH, RDE: 1600 r/min)(A), RDE polarization profiles of Mn/Fe⁃HIB⁃MOF for various rotation speeds(the insert: the respective K—L profiles for different voltages)(B), RRDE⁃calculated electron transfer numbers and HO2- yields during ORR for Mn/Fe⁃HIB⁃MOF(C), ORR polarization profiles of Mn/Fe⁃HIB⁃MOF before and after 10000 cycles(the inset: the respective CVs)(D)[102]Copyright 2019, the Royal Society of Chemistry.
Fig.20 Initial structure and structures after the adsorption of hydroxyl OH*, oxyl O*, and hydroperoxyl OOH* intermediates on Mn/Fe⁃HIB⁃MOF(inset: active sites with elements and Arabic numbers)(A), Volcano profiles for OER(B) and ORR(C) for Mn⁃HIB⁃MOF, Fe⁃HIB⁃MOF, and Mn/Fe⁃HIB⁃MOF catalysts[102]Copyright 2019, the Royal Society of Chemistry.
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