高等学校化学学报 ›› 2022, Vol. 43 ›› Issue (11): 20220544.doi: 10.7503/cjcu20220544
收稿日期:
2022-08-17
出版日期:
2022-11-10
发布日期:
2022-09-23
通讯作者:
于然波
E-mail:ranboyu@ustb.edu.cn
基金资助:
WANG Zumin1,2, MENG Cheng1, YU Ranbo1,3()
Received:
2022-08-17
Online:
2022-11-10
Published:
2022-09-23
Contact:
YU Ranbo
E-mail:ranboyu@ustb.edu.cn
Supported by:
摘要:
过渡金属磷化物因其优异的催化性能成为最有可能取代贵金属的廉价电催化分解水制氢催化材料, 对其进行元素掺杂将有望大幅提升其活性和稳定性. 本文综合评述了近年来通过掺杂改性手段调节过渡金属磷化物性能的相关研究. 讨论了元素种类(金属掺杂、 非金属掺杂、 共掺杂)、 元素数量(单元素掺杂、 多元素掺杂、 高熵化)和掺杂位置等因素对过渡金属磷化物电子结构的影响; 并从实验和理论相结合的角度, 分析了掺杂元素对氢吸附强度、 水吸附解离及电荷转移传输等方面的作用规律, 获得了掺杂结构-电子结构-析氢反应催化性能间的构效关系. 最后, 讨论并提出了相关研究存在的挑战和未来的研究方向.
中图分类号:
TrendMD:
王祖民, 孟程, 于然波. 过渡金属磷化物析氢催化剂的掺杂调控. 高等学校化学学报, 2022, 43(11): 20220544.
WANG Zumin, MENG Cheng, YU Ranbo. Doping Regulation in Transition Metal Phosphides for Hydrogen Evolution Catalysts. Chem. J. Chinese Universities, 2022, 43(11): 20220544.
Fig.2 A calculated volcano plot(A)[39], the LSVs normalized to the electrochemical active surface area(ECSA)(B), activity volcano for the HER showing the ECSA normalized current density at η = 100 mV as a function of ΔGH(C)[40](A) Copyright 2010, American Chemical Society; (B, C) Copyright 2015, Royal Society of Chemistry.
Fig.3 DFT calculationsConfigurations(A) and the calculated free-energy diagram(B) of Ni-CoP, Mn-CoP, Fe-CoP and CoP[44], Copyright 2019, Elsevier; (C) Calculated densities of states(DOS) of Ni0.1Co0.9P and CoP with the Fermi level aligned at 0 eV[45], Copyright 2018, Wiley Online Library.
Fig.4 Top view of the H adsorbed on Ni hollow site(A), relationship between hydrogen adsorption free energy(ΔGH*) and charge transfer to the surface(ΔQ) of M?Ni2P[(M=Ti, Nb, V, Li, Cr, Na, Mn, Fe, Co, Sn, and Pb), the insets: charge density difference plots of Pb, Co, Cr and Ti?Ni2P, respectively](B), relationship between εd and ΔQ of M?Ni2P(C), corresponding schematic illustration of bond formation of Ni2P and M?Ni2P(D), relationship between ΔGH* and εd of M?Ni2P(E), and the corresponding overpotentials of Ni2P, M?Ni2P, and Pt/C at a current density of 10 mA/cm2(F)[48]Copyright 2021, Elsevier.
Fig.5 TEM images(A), polarization curves(B), Tafel slopes(C) and Nyquist plots(D) of FeP/Ti, Co?FeP/Ti, Ni?FeP/Ti, and Mn?FeP/Ti[23]Copyright 2020, Elsevier.
Fig.6 Reaction energy diagram of water dissociation into H* and OH* on the CoP(211), CoMoP(112), CoMoP(112)?Pv and Pt(111) surfaces(A)[54], free energy diagram for H2O activation(cleavage of O—H bonds of H2O molecules) of CoP and Co0.75V0.25P(B)[52](A) Copyright 2020, Elsevier; (B) Copyright 2020, Springer Nature.
Fig.7 CoP(111) surface model with or without a second transition metal(M′) substitution(A), schematic energy bands of individual water HOMO and M′ d orbital on M′?substituted CoP(111) surface(εF: the Fermi level)(B), the crystal orbital Hamilton population(COHP) analysis for the Co2—O bond on CoP(111) surface and the Cr—O bond on the Cr—CoP(111) surface(all of the energies shown relative to the Fermi level εF)(C), the relative energy profiles and the simplified surface structures of the various reaction species along the alkaline Volmer reaction pathway on CoP(111) and Cr—CoP(111) surfaces(D), the COHP analysis for the Co2—H bond in CoP(111) and the Cr—H bond in Cr—CoP(111)(E), the relative energy profiles and the simplified surface structures of the various reaction species along the alkaline Heyrovsky reaction pathway on CoP(111) and Cr—CoP(111) surfaces with an already?adsorbed H(F), the calculated water adsorption free energy(ΔG?H2O) vs. Pun(G), the calculated water dissociation barrier(Ea) of Volmer step vs. Pun(H), trends in η@10 mA/cm2 for alkaline HER shown as a function of Pun(I)[55](A) Blue, orange, and yellow circles represent Co, M′(or Co), and P atoms, respectively; the structures at the upper and lower right are CoP3(H2O) and M′P3(H2O) tetrahedrals, respectively. Copyright 2020, Elsevier.
Fig.8 Hydrogen adsorption on the(011) surfaces of CoP(A), Mo0.125Co0.875P(B), Mo0.25Co0.75P(C), Mo0.375Co0.625P(D), Mo0.5Co0.5P(E), and on the surface of Pt(111)(F), free energy diagram of the hydrogen evolution reaction over Mo x Co1-x P(011) and Pt(111)(G)[56]Copyright 2019, Royal Society of Chemistry.
Fig.9 Schematic structural representations for hydrogen adsorption at CoP(A), Fe0.25Co0.75P(B), Fe0.33Co0.66P(C), and Fe0.5Co0.5P(D), free energy diagram of HER under favorable Co site of hydrogen coverage on surface of Fe x Co1–x P(E)[57], Gibbs free energy image of (Ni x Fe1-x )2P(x = 0, 0.5, 0.75, 0.83, 1)(F)[58](A)—(E) Copyright 2016, American Chemical Society; (F) Copyright 2019, Royal Society of Chemistry.
Fig.10 TEM(A), and HRTEM(B) images of the Cr?doped FeNi?P/NCN, adsorption energies of H, H2O, and OH on the FeNi?P and Cr?doped FeNi?P surface for HER(C)[61]Copyright 2019, Wiley Online Library.
Fig.11 Fe L3?edge XANES(A), Fe2p XPS(B) spectra of FeCoP and FeCoRuP, Nyquist plots of FeCoP, FeCoRuP, and commercial 20% Pt/C(C)[62]Copyright 2020, Royal Society of Chemistry.
Fig.12 Corresponding overpotentials at a current density of 10 mA/cm2 and the active site density(ASD) with different mol/L doping amounts for V?(A) and Cr?FeCoP(B)[65]Copyright 2020, Royal Society of Chemistry.
Fig.13 Synthesis process of high?entropy metal phosphide(HEMP) NiCoFeMnCrP NPs for electrocatalytic water splitting through the sol?gel method and calcination reduction strategy(A), the evolution of the crystal structures of NiP, NiCoP, NiCoFeP, NiCoFeMnP and NiCoFeMnCrP NP(B), XRD patterns of NiP, NiCoP, NiCoFeP, NiCoFeMnP and NiCoFeMnCrP NPs(inset: crystal structure model)(C), HER LSV curves(D), and overpotentials at 10 mA/cm2(E) of the different electrocatalysts [70]Copyright 2021, Royal Society of Chemistry.
Catalyst | Electrolyte | Overpotential/mV | Tafel slop/ (mV·dec?1) | TOF/s?1 | Stability | Ref. |
---|---|---|---|---|---|---|
Ni?CoP | 0.5 mol/L H2SO4 | 144(10 mA/cm2) | 52 | 0.1(164 mV) | 21 h | [ |
Fe?CoP | 1 mol/L KOH | 92(10 mA/cm2) | 71 | 21 h | [ | |
Fe?CoP | 0.5 mol/L H2SO4 | 198(10 mA/cm2) | 68 | [ | ||
Ni?CoP | 1 mol/L KOH | 173(10 mA/cm2) | 87 | [ | ||
Mn?CoP | 0.5 mol/L H2SO4 | 198(10 mA/cm2) | 65 | [ | ||
Al?CoP/CC | 1 mol/L KOH | 173(10 mA/cm2) | 76 | [ | ||
Ni?CoP | 1 mol/L PBS | 125(10 mA/cm2) | 103 | 0.24 ?(125 mV) | >20 h(1000 cycles) | [ |
Zn?CoP | 0.5 mol/L H2SO4 | 39(10 mA/cm2) | 39 | 22 h | [ | |
V?CoP | 1 mol/L KOH | 46(10 mA/cm2)/115(100 mA/cm2) | 58 | 24 h | [ | |
Al?CoP/CC | 0.5 mol/L H2SO4 | 23(10 mA/cm2) | 43 | 0.27(100 mV) | >80 h(1000 cycles) | [ |
Cr?Ni2P | 0.5 mol/L H2SO4 | 56(10 mA/cm2) | 56 | [ | ||
Mn?Ni2P | 0.5 mol/L H2SO4 | 46(10 mA/cm2) | 53 | [ | ||
Fe?Ni2P | 0.5 mol/L H2SO4 | 31(10 mA/cm2) | 52 | 0.282(100 mV) | 20 h | [ |
Co?Ni2P | 0.5 mol/L H2SO4 | 31(10 mA/cm2) | 47 | 0.381(100 mV) | 20 h | [ |
Mn?FeP | 0.5 mol/L H2SO4 | 175(10 mA/cm2) | 103.6 | [ | ||
Co?FeP | 0.5 mol/L H2SO4 | 126(10 mA/cm2) | 63.6 | [ | ||
Ni?FeP | 0.5 mol/L H2SO4 | 169(10 mA?cm-2) | 86.9 | [ |
Table 1 HER performance for different metal doped catalysts
Catalyst | Electrolyte | Overpotential/mV | Tafel slop/ (mV·dec?1) | TOF/s?1 | Stability | Ref. |
---|---|---|---|---|---|---|
Ni?CoP | 0.5 mol/L H2SO4 | 144(10 mA/cm2) | 52 | 0.1(164 mV) | 21 h | [ |
Fe?CoP | 1 mol/L KOH | 92(10 mA/cm2) | 71 | 21 h | [ | |
Fe?CoP | 0.5 mol/L H2SO4 | 198(10 mA/cm2) | 68 | [ | ||
Ni?CoP | 1 mol/L KOH | 173(10 mA/cm2) | 87 | [ | ||
Mn?CoP | 0.5 mol/L H2SO4 | 198(10 mA/cm2) | 65 | [ | ||
Al?CoP/CC | 1 mol/L KOH | 173(10 mA/cm2) | 76 | [ | ||
Ni?CoP | 1 mol/L PBS | 125(10 mA/cm2) | 103 | 0.24 ?(125 mV) | >20 h(1000 cycles) | [ |
Zn?CoP | 0.5 mol/L H2SO4 | 39(10 mA/cm2) | 39 | 22 h | [ | |
V?CoP | 1 mol/L KOH | 46(10 mA/cm2)/115(100 mA/cm2) | 58 | 24 h | [ | |
Al?CoP/CC | 0.5 mol/L H2SO4 | 23(10 mA/cm2) | 43 | 0.27(100 mV) | >80 h(1000 cycles) | [ |
Cr?Ni2P | 0.5 mol/L H2SO4 | 56(10 mA/cm2) | 56 | [ | ||
Mn?Ni2P | 0.5 mol/L H2SO4 | 46(10 mA/cm2) | 53 | [ | ||
Fe?Ni2P | 0.5 mol/L H2SO4 | 31(10 mA/cm2) | 52 | 0.282(100 mV) | 20 h | [ |
Co?Ni2P | 0.5 mol/L H2SO4 | 31(10 mA/cm2) | 47 | 0.381(100 mV) | 20 h | [ |
Mn?FeP | 0.5 mol/L H2SO4 | 175(10 mA/cm2) | 103.6 | [ | ||
Co?FeP | 0.5 mol/L H2SO4 | 126(10 mA/cm2) | 63.6 | [ | ||
Ni?FeP | 0.5 mol/L H2SO4 | 169(10 mA?cm-2) | 86.9 | [ |
Fig.14 Top views of the optimized geometric structures for Co2P and N—Co2P(Blue ball: Co, pink ball: P, grey ball: N)(A), density of States of Co2P and N—Co2P(B), DFT?calculated ΔGH*for Co2P(201) and N—Co2P(201) surface(C)[79]Copyright 2021, Elsevier.
Fig.15 Free?energy diagram for HER(A), and iR?corrected HER polarization curves(B) of B?CoP/CNT, CoP/CNT, phosphatized CNT catalysts and commercialized Pt/C(20%)[81]Inset of (B): the corresponding HER overpotential required for j=10 mA/cm2. Copyright 2020, Wiley Online Library.
Catalyst | Electrolyte | Overpotential/mV | Tafel slop/ (mV·dec?1) | TOF/s?1 | Stability | Ref. |
---|---|---|---|---|---|---|
S?Ni5P4 NPA/CP | 0.5 mol/L H2SO4 | 56(10 mA/cm2) | 43.6 | 0.11(100 mV) | 100 h | [ |
105(100 mA/cm2) | ||||||
S?Co2P@NF | 1 mol/L KOH | 105(10 mA/cm2) | 89 | 0.127(350 mV) | 20 h | [ |
192(100 mA/cm2) | ||||||
S?CoP@NF | 1 mol/L KOH | 109(10 mA/cm2) | 79 | 0.23(350 mV) | 20 h | [ |
185(100 mA/cm2) | ||||||
N?Co2P/CC | 0.5 mol/L H2SO4 | 27(10 mA/cm2) | 45 | 3000 cycles | [ | |
1 mol/L KOH | 34(10 mA/cm2) | 51 | ||||
1 mol/L PBS | 42(10 mA/cm2) | 68 | ||||
N?Co2P | 1 mol/L KOH | 58(10 mA/cm2) | 75 | 5000 cycles | [ | |
N?CoP | 0.5 mol/L H2SO4 | 42(10 mA/cm2) | 41.2 | 0.0199(50 mV) | 5000 cycles, 20 h | [ |
O?CoP | 1 mol/L KOH | 98(10 mA/cm2) | 59.9 | 15 h, 2000 cycles | [ | |
B?CoP/CNT | 0.5 mol/L H2SO4 | 39(10 mA/cm2) | 50 | 5000 cycles, 100 h | [ | |
1 mol/L KOH | 56(10 mA/cm2) | 69 | ||||
1 mol/L PBS | 79(10 mA/cm2) | 80 | ||||
Se?CoP | 1 mol/L KOH | 41(10 mA/cm2) | 46 | 0.158(200 mV) | 2000 cycles | [ |
NiP1.93Se0.07/CP | 0.5 mol/L H2SO4 | 84(10 mA/cm2) | 41 | ca. 0.8(100 mV) | 14 h | [ |
Table 2 HER performance for different non-metal doped catalysts
Catalyst | Electrolyte | Overpotential/mV | Tafel slop/ (mV·dec?1) | TOF/s?1 | Stability | Ref. |
---|---|---|---|---|---|---|
S?Ni5P4 NPA/CP | 0.5 mol/L H2SO4 | 56(10 mA/cm2) | 43.6 | 0.11(100 mV) | 100 h | [ |
105(100 mA/cm2) | ||||||
S?Co2P@NF | 1 mol/L KOH | 105(10 mA/cm2) | 89 | 0.127(350 mV) | 20 h | [ |
192(100 mA/cm2) | ||||||
S?CoP@NF | 1 mol/L KOH | 109(10 mA/cm2) | 79 | 0.23(350 mV) | 20 h | [ |
185(100 mA/cm2) | ||||||
N?Co2P/CC | 0.5 mol/L H2SO4 | 27(10 mA/cm2) | 45 | 3000 cycles | [ | |
1 mol/L KOH | 34(10 mA/cm2) | 51 | ||||
1 mol/L PBS | 42(10 mA/cm2) | 68 | ||||
N?Co2P | 1 mol/L KOH | 58(10 mA/cm2) | 75 | 5000 cycles | [ | |
N?CoP | 0.5 mol/L H2SO4 | 42(10 mA/cm2) | 41.2 | 0.0199(50 mV) | 5000 cycles, 20 h | [ |
O?CoP | 1 mol/L KOH | 98(10 mA/cm2) | 59.9 | 15 h, 2000 cycles | [ | |
B?CoP/CNT | 0.5 mol/L H2SO4 | 39(10 mA/cm2) | 50 | 5000 cycles, 100 h | [ | |
1 mol/L KOH | 56(10 mA/cm2) | 69 | ||||
1 mol/L PBS | 79(10 mA/cm2) | 80 | ||||
Se?CoP | 1 mol/L KOH | 41(10 mA/cm2) | 46 | 0.158(200 mV) | 2000 cycles | [ |
NiP1.93Se0.07/CP | 0.5 mol/L H2SO4 | 84(10 mA/cm2) | 41 | ca. 0.8(100 mV) | 14 h | [ |
Fig.16 HER polarization curve normalized by electrochemical double?layer capacitance(A), corresponding HER path and energy diagram on the (011) surface of pure CoP and Cu, O?doped CoP(B), structural models of *H?OH and *H adsorption free energies calculated(blue: Co, green: Cu, pink: P, red: O, gray: H)(C)[84]Copyright 2018, American Chemical Society.
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