Acta Phys. -Chim. Sin. ›› 2023, Vol. 39 ›› Issue (12): 2302049.doi: 10.3866/PKU.WHXB202302049
Special Issue: Energy and Environmental Catalysis
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Function of Electron Spin Effect in Electrocatalysts
Jingxue Li1,2, Yue Yu1,2, Siran Xu1,2, Wenfu Yan3, Shichun Mu4, Jia-Nan Zhang1,2,*(
)
- 1 College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China
2 Key Laboratory of Advanced Energy Catalytic and Functional Materials Preparation, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450012, China
3 State Key Laboratory of Inorganic Synthesis and Preparation Chemistry, School of Chemistry, Jilin University, Changchun 130012, China
4 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
-
Received:2023-02-27Accepted:2023-03-20Published:2023-03-28 -
Contact:Jia-Nan Zhang E-mail:zjn@zzu.edu.cn -
Supported by:the National Natural Science Foundation of China(U22A20107);the National Natural Science Foundation of China(U1967215);the Distinguished Young Scholars Innovation Team of Zhengzhou University(32320275);the Academic Degrees & Graduate Education Reform Project of Henan Province(2021SJGLX093Y);the Science and Technology Research Support Plan in Henan Province(222301420001)
Cite this article
Jingxue Li, Yue Yu, Siran Xu, Wenfu Yan, Shichun Mu, Jia-Nan Zhang. Function of Electron Spin Effect in Electrocatalysts[J]. Acta Phys. -Chim. Sin. 2023, 39(12), 2302049. doi: 10.3866/PKU.WHXB202302049
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Fig 1
(a) Spin states of common oxygen species. (b) Selective Spin Electron Transfer in ORR 60. (b) Adapted with permission from Ref. 60, Copyright 2020, Wiley-VCH."
Fig 2
(a) S-doped Fe-N-C induced Fe central spin polarization 74. (b) Distribution of electron spin states ofLaCoO3 in (100) (110) (111) configuration 76. (c) Schematic diagram of polarized electron generation underconstant magnetic field 77. (d) Schematic diagram of active sites of magnetic effect precision heating catalyst 78. (a) Adapted with permission from Ref. 74, Copyright 2021, Wiley-VCH. (b) Adapted with permission from Ref. 76, Copyright 2011, IOP Pub. (c) Adapted with permission from Ref. 77, Copyright 2021, Nature Publishing Group. (d) Adapted with permission from Ref. 78, Copyright 2021, Nature Publishing Group."
Fig 3
(a) Schematic diagram of the first electron transfer step of ferromagnetic oxide and (b) paramagnetic oxide inORR 85. (c) Schematic diagram of OER spin exchange mechanism 77. (d) The relationship between the OER (blue) andORR (yellow) activities of perovskite and the eg orbital magnetization was predicted 86. (a–b) Adapted with permission from Ref. 85, Copyright 2017, Chemistry Europe. (c) Adapted with permission from Ref. 77, Copyright 2021, Nature Publishing Group. (d) Adapted with permission from Ref. 86, Copyright 2017, Royal Society of Chemistry."
Fig 4
(a) Schematic diagram of quantum spin exchange interaction. (b, c)QSEIshellopen energy/space diagram of antiferromagnetic or ferromagnetic catalyst. (d) Electronic description of antisymmetric wave function 93.(e) Density of states from FeOOH and NixFe1−xOOH. (f) Spin electron transfer route of FeOOH and NixFe1−xOOH 94. (a–d) Adapted with permission from Ref. 93, Copyright 2021, American Chemical Society. (e–f) Adapted with permission from Ref. 94, Copyright 2020, Wiley-VCH."
Fig 5
(a) 57Fe Mössbauer spectra of Fe, Mn/N-C catalyst at room temperature. (b, c) Spin states of Fe3+in Fe, Mn/N-C and Fe/N-C catalysts 102. (d) Comparison diagram of pyrrole-N and pyridine-N contents in Fe-N5-LS, Fe-N4-HS andFe-N3-HS samples. (e) Hysteresis loop of Fe-N-C powder at room temperature (300 K). (f) LSV curve of differentsamples at 900 r∙min−1 104. (g) The electronic transition of Co from low spin to high spin. (h) Linear volt-amperecurves of MCN electrode with and without magnetic field. (i) Tafel diagrams of ORR activity of different samples 105. (a–c) Adapted with permission from Ref. 102, Copyright 2021, Nature Publishing Group. (d–f) Adapted with permission from Ref. 104, Copyright 2022, Wiley-VCH. (g–i) Adapted with permission from Ref. 105, Copyright 2020, Wiley-VCH."
Fig 6
57Fe Mössbauer spectra of Fe0.5 (a) at the initial state and (b) after 50 h battery operation at 0.5 V. (c) Initial polarization curve and final polarization curve108. (d, e) 57Fe Mössbauer spectra of Fe-AC and Fe-AC-CVD samples.(f) D1 and D2 site content map of two catalysts. (g) Possible structural change pathway from S1 to S2. The gray, blue, white and orange spheres represent C, N, H and Fe atoms respectively. Ef stands for free energy 106. (a–c) Adapted with permission from Ref.108, Copyright 2021, Nature Publishing Group. (d–g) Adapted with permission from Ref. 106, Copyright 2022, Nature Publishing Group."
Fig 7
(a) Schematic diagram of electron interaction in dxy orbit of NiFe-LDHs and Cu-NiFe-LDHs.(b) Cu0-Ni6Fe2-LDHs and Cu1-Ni6Fe2-LDHs of VSM curve. (c) Overpotential curves of Cu0-Ni6Fe2-LDHs andCu1-Ni6Fe2-LDHs under magnetic field 111. (d) Evolution diagram of Co3+ spin state and Co-O-Co spinchannel in the process of raising Co spin state. (e) The CV curve of ZnCo2O4 sample 115.(f) Schematic diagram of the mechanism of iodine cation and anion double doping in I-BSCF 116. (a–c) Adapted with permission from Ref. 111, Copyright 2022, American Chemical Society. (d–e) Adapted with permission from Ref. 115, Copyright 2022, Wiley-VCH. (f) Adapted with permission from Ref. 116, Copyright 2022, Elsevier."
Fig 8
(a) Schematic diagram of N2 bonding with transition metal. (b) Schematic diagram of FeMoPPc magnetic susceptibility and electron orbit layout. (c) 57Fe Mössbauer spectra of FeMoPPc at room temperature. (d) LSV curves inN2 and Ar atmosphere under alkaline condition 120. (e) M–H magnetization curves of TiO2, Fe: TiO2 and F-Fe: TiO2.(f) EPR spectra of TiO2, Fe: TiO2 and F-Fe: TiO2. (g) Electrochemical impedance spectrum of the sample 121.(h) The spin resolution density diagram of Rh/graphene. The yellow area represents charge accumulation.(i) NH3 yield of samples at different voltages 122. (a–d) Adapted with permission from Ref. 120, Copyright 2021, Wiley-VCH. (e–g) Adapted with permission from Ref. 121, Copyright 2022, Elsevier. (h–i) Adapted with permission from Ref. 122, Copyright 2021, Elsevier."
Fig 9
(a) Comparison of the density of states of different samples. (b) Comparison of the binding energies of thekey intermediates of HER and CO2RR on different samples 126. (c) Comparison diagram of catalyst limiting potential.(d) CO2 RR adsorption energy and catalyst magnetic moment volcano diagram 130. (e) Free energy diagram ofCO2 reduction to CH3OH and corresponding intermediates on Fe-N4 porphyrin and Fe-N2S2 porphyrin 131.(f) Schematic diagram of Ni/Cu-N-C catalyst synthesis. (g) Schematic diagram of Fermi energy level of Ni 3d orbit 132. (a–b) Adapted with permission from Ref. 126, Copyright 2021, Wiley-VCH. (c–d) Adapted with permission from Ref. 130, Copyright 2022, Elsevier. (e) Adapted with permission from Ref. 131, Copyright 2021, Wiley-VCH. (f–g) Adapted with permission from Ref. 132, Copyright 2022, American Chemical Society."
Fig 10
Advanced characterization technology ofelectron spin-state: X-ray absorption spectroscopy (XAS), X-ray emission spectroscopy (XES), vibrating sample magnetometer (VSM), Mössbauer spectroscopy, electron paramagnetic resonance (EPR)."
Fig 11
Simulated calculation method to analyze catalyst spin. (a) W-NiS0.5Se0.5 spin-polarized projection density of states calculation 156. (b) NixFe1−xOOH spin densitydiagram 94. (c) ORR step diagram of CoBDC FcCA 157(d) Computational stability-activity relationshipdiagram of Fe-N-C catalysts with different-spin states 158. (a) Adapted with permission from Ref. 156, Copyright 2022, Wiley-VCH. (b) Adapted with permission from Ref. 94, Copyright 2020, Wiley-VCH. (c) Adapted with permission from Ref. 157, Copyright 2022, American Chemical Society. (d) Adapted with permission from Ref. 158, Copyright 2022, American Chemical Society."
Fig 12
Challenges and perspectives forspin effect in electrocatalysis."
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