Enhancing the performance of platinum group metal-based electrocatalysts through nonmetallic element doping

doi:10.1016/S1872-2067(23)64569-3

Abstract

Abstract:

abstract: Platinum group metal (PGM) catalysts have been well recognized as one of the best catalysts towards energy conversion and storage devices, such as fuel cells and water electrolyzers. Nevertheless, their commercial applications are strictly limited by the unsatisfactory catalytic activity and stability. Recently, nonmetallic (H, B, C, N, P, S, etc.) atoms doping is explored to be an efficient strategy to optimize the catalytic activity and durability of PGM-based catalysts via precisely electronic and coordination structure modulation, thus arising tremendous attention. However, systematical discussions on this topic is still lacking. In this review, the representative progresses of nonmetal elements doped PGM-based electrocatalysts for different electrocatalytic reactions are summarized. Firstly, this review discusses the key factors that affect the activity and stability of the catalysts, and introduces the basic principles of nonmetal-doping for improving the performance of PGM-based catalysts. Secondly, advanced characterization techniques and theoretical calculations are highlighted respectively for revealing the activity enhancement mechanism. Then the synthesis methods to incorporate the nonmetals are listed, intending to provide inspirations for the future design of materials. The promising modification strategies for tuning the active species are further proposed. Afterwards, an overview of nonmetal-doped PGM-based catalysts is provided for the electrocatalytic applications, with an emphasis on revealing the structure-performance relationship. Finally, further developments and challenges involving synthesis, mechanism analysis, new materials as well as reactions, stability issues and practical applications are outlined, aiming to promote the in-depth research on advanced PGM-based catalysts.

Key words: Electrocatalysis, Nonmetal doping, Platinum group metal-based catalyst, Oxygen reduction, ydrogen evolution

Yiping Li, Tanyuan Wang, Zhangyi Yao, Qi’an Chen, Qing Li. Enhancing the performance of platinum group metal-based electrocatalysts through nonmetallic element doping[J]. Chinese Journal of Catalysis, 2024, 56: 51-73.

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Figures/Tables 27

Fig. 1. Representative achievements in nonmetal doped PGM-based catalysts toward various electrocatalytic reactions.

Fig. 2. Mechanisms on tuning the activity of PGM-based electrocatalysts through nonmetallic element doping. (a) The effect of strain on the width and position of the d band for PGM. (b) The microstrain, represented as the change in peak broadening of WAXS patterns. And the peak position is related to macrostrain or global strain. Reprinted with permission from Ref. [71]. Copyright 2018, Springer Nature. (c) The influence of ligand effect on the εd of PGM. (d) Illustration of synergistic effect, where nonmetals and PGMs both act as adsorption sites for different intermediates. The green and pink balls represent PGM and nonmetal atoms respectively.

Fig. 3. (a) The correlation between the dissolution amounts of metals during oxidation process and the cohesive energy (Ecoh). Reprinted with permission from Ref. [102]. Copyright 2021, Wiley-VCH. (b) Total bond energies of 32-metal-atom supercell with FCC structure from the fitting (y-axis) vs. the DFT-calculated total bond energies used for the fit (x-axis). The more negative energy end (?185 eV) corresponds the composition with high concentration of interstitial carbon. Reprinted with permission from Ref. [105]. Copyright 2021, Elsevier.

Fig. 4. (a) Relationship between work functions of metals and their corresponding dissolution potential. Reprinted with permission from Ref. [113]. Copyright 2022, Electrochemical Society. (b) Relationship between the work functions and carbon content. Reprinted with permission from Ref. [116]. Copyright 2021, Electrochemical Society.

Table 1 The summary of properties for each doped nonmetal.

Nonmetal	Located position in the lattice of PGMs	Advantage	Disadvantage
H	interstitial sites	good electron donor; wide doping concentration range	unstable; introducing unfavorable tensile strain for certain reactions
B	interstitial sites	good electron donor; flexible structure adjustment	introducing unfavorable tensile strain for certain reactions
C	interstitial sites	strong C-metal bonds; inhibiting the dissolution of metal	forming compounds with metal, resulting in phase separation
N	interstitial or substitutional sites	strong N-metal bonds; inhibiting the dissolution of metal	forming compounds with metal, resulting in phase separation
P	interstitial or substitutional sites	causing lattice distortion and optimized structure; favorable for OH adsorption	may be oxidized and then dissolve
S	interstitial or substitutional sites	strong interaction with PGMs; inhibiting the dissolution of metal	may poison active sites; limited doping pattern

Fig. 5. (a) Differential phase contrast images of PdHx nanoparticle, where the brighter atoms represent Pd atoms, while the darker and smaller atoms represent H atoms. Reprinted with permission from Ref. [46]. Copyright 2020, Wiley-VCH. (b) Ptychographic phase image of B doped Pd nanoparticle after aberration correction, where the red balls refer to the B atoms. Reprinted with permission from Ref. [126]. Copyright 2019, American Chemical Society.

Fig. 6. (a) Accordingly in-situ XPDF from room temperature to the elevated temperature, after zoning up in the range of 2-6 ?. Reprinted with permission from Ref. [126]. Copyright 2019, American Chemical Society. (b) In-situ XRD of Pd@Ru under different gas atmospheres. Reprinted with permission from Ref. [127]. Copyright 2023, American Chemical Society.

Fig. 8. (a) Reaction process schematic diagram of PtNiP NWs in alkaline condition. Reprinted with permission from Ref. [62]. Copyright 2021, Elsevier. (b) Reaction path ways of P-Rh for alkaline HER and HOR. Reprinted with permission from Ref. [132]. Copyright 2020, Royal Society of Chemistry.

Fig. 9. Strategies for introducing nonmetals into PGM-based catalysts.

Fig. 10. (a) The correlation between the N contents and NH3 pressure in N doped PtCo catalysts. Reprinted with permission from Ref. [136]. Copyright 2021, American Chemical Society. (b) Schematic of the high-temperature pyrolysis synthesis of P,Mo-Ru@P-doped porous carbon. Reprinted with permission from Ref. [29]. Copyright 2022, Wiley-VCH. (c) Schematic of the Schematic of the wet chemical synthesis of Pd-B alloy mesoporous nanospheres. Reprinted with permission from Ref. [139]. Copyright 2022, Royal Society of Chemistry. (d) Schematic of hydrogen dissolving in Au@Pd@Ru catalysts during hydrogen oxidation reaction. Reprinted with permission from Ref. [127]. Copyright 2023, American Chemical Society.

Fig. 11. (a) Scheme for the synthesis; High-resolution XPS spectra of Ag 3d spectra (b) and Ni 2p3/2 spectra (c). Reprinted with permission from Ref. [144]. Copyright 2021, American Chemical Society. (d) Rh-Pd solid-state miscibility gap. (e) The schematic illustration of the formation energy of 2D RhPd alloy and alloy hydride. Reprinted with permission from Ref. [141]. Copyright 2020, American Chemical Society.

Fig. 12. HR-TEM image (a) and Nyquist plot (b) of a/c-RuB aerogel. Reprinted with permission from Ref. [147]. Copyright 2023, Wiley-VCH. (c) The electronic local function of B-Rh@CN. Reprinted with permission from Ref. [138]. Copyright 2023, Elsevier. (d) The differential charge density distributions between P,Mo-Ru clusters and PC. Red represents positive charges and green represents negative charges. (e) Differential charge density distributions for selected single Ru atom in P,Mo-Ru cluster. Reprinted with permission from Ref. [29]. Copyright 2022, Wiley-VCH.

Fig. 13. The mechanism for ORR, white: surface PGM; pink: O; purple: H.

Table 2 Summary of nonmetal doped PGM-based catalysts for ORR.

Catalyst	Nonmetal source	Synthesis method	Electrolyte	MA (A mg^-1) at half cell test	Maximum power density (mA cm^-2) at MEA	Ref.
C-doped PdMo bimetallene	glucose	wet chemical reduction	0.1 mol L^-1 KOH	7.013	—	[47]
B-doped Pd nanoparticles	DMAB	wet chemical reduction	0.1 mol L^-1 KOH	2.38	—	[39]
B-doped Pt nanoparticles	DMAB	wet chemical reduction	0.1 mol L^-1 HClO₄	0.25	1.6 for H₂-O₂	[30]
P-doped Pt nanoparticles	NaH₂PO₂	wet chemical reduction	0.1 mol L^-1 HClO₄	1	1.06 for H₂-air	[154]
N-doped Intermetallic PtNi nanoparticles	NH₃	chemical vapor deposition	0.1 mol L^-1 HClO₄	1.83	—	[40]
N-doped PtCo nanoparticles	NH₃ and N₂	chemical vapor deposition	0.1 mol L^-1 HClO₄	more than 0.7	—	[136]
N-doped Pt nanoparticles	NH₃	chemical vapor deposition	0.1 mol L^-1 HClO₄	0.10	1.2 for H₂-air	[42]

Fig. 14. (a) Cross section of the P-Pt(111) model showing concave site (site 3 and 4) of surface Pt atoms. (b) DFT calculation models of P doped Pt/C, which indicates that the OH binding energy on Pt site 4 decreased by 0.12 eV relative to Pt(111), close to the predicted optimal value; Gold: Pt; blue: surface Pt; green: P; red: O; and white: H. (c) Polarization curves of P doped Pt/C in H2-air fuel cells. Reprinted with permission from Ref. [154]. Copyright 2021, American Chemical Society. (d) Ni K-edge extended X-ray absorption fine structure spectrum at 0.42 V with a first-shell fit, indicating the formation of Ni?N bond. Reprinted with permission from Ref. [40]. Copyright 2020, American Chemical Society.

Fig. 15. (a) Bader charges and geometrical configurations of oxygen atoms adsorbed on the modeled Pt (111) surfaces with B doping at B coverage = 0.75. The blue, orange, and red balls represent Pt, B, and O atoms, respectively. (b) Polarization curves of B doped Pt/C and commercial Pt/C in H2-O2 fuel cells before and after ADT. Reprinted with permission from Ref. [30]. Copyright 2022, American Chemical Society.

Fig. 16. (a) The synthetic process. (b) DFT calculated stable configuration of C-doped PdMo alloy, wherein Er represents the energy of removing a Mo atom from the system. (c) MA retention of C-doped PdMo, pure PdMo bimetallene and commercial Pt/C. Reprinted with permission from Ref. [47]. Copyright 2022, American Chemical Society.

Fig. 17. The mechanism in acid (a) and alkaline (b) environment for HER, green: surface PGM.

Table 3 Summary of nonmetal doped PGM-based catalysts for HER/HOR.

Catalyst	Nonmetal source	Synthesis method	Electrolyte	Reaction	Performance (HER: η₁₀ (mV), HOR: j₀ (mA cm⁻²))	Ref.
P doped Pt nanodendrites	NaH₂PO₂	wet chemical reduction	0.5 mol L^‒1 H₂SO₄	HER	13.3	[85]
S-Doped RuP @N,P, S-Doped carbon	cyclotriphosphazene- co-4,4′-sulfonyldiphenol	high temperature pyrolysis process	1 mol L^‒1 KOH	HER	92	[51]
P,Mo-Ru @P-doped porous carbon	phosphomolybdic acid hydrate	high temperature pyrolysis process	1 mol L^‒1 KOH	HER	21	[29]
P-Ru/C	TOPO	wet chemical reduction	0.1 mol L^‒1 KOH	HER/HOR	31 for HER, 0.72 for HOR	[143]
PtNiP nanowires	phosphorus powder	wet chemical reduction	1 mol L^‒1 KOH	HER	9	[62]
P-doped Rh nanoparticles	TOP	wet chemical reduction	1 mol L^‒1 KOH for HER, 0.1 mol L^‒1 KOH for HOR	HER/HOR	11 for HER, 0.683 for HOR	[132]
B-Rh@NC	H₃BO₃	high temperature pyrolysis process	full pH range	HER	26 in 1.0 mol L^‒1 KOH, 43 in 0.5 mol L^‒1 H₂SO₄, 70 in 1.0 mol L^‒1 PBS	[138]
B doped Pd nanoparticles	DMAB	wet chemical reduction	1 mol L^‒1 KOH	HER	38	[38]
IrPdH nanodendrites	ethanol	wet chemical reduction	full pH range	HER	14, 25, and 60 respectively in 0.5 mol L^‒1 H₂SO₄, 1 mol L^‒1 KOH, and 1 mol L^‒1 PBS electrolyte	[49]
RhPdH 2D Bimetallene Nanosheets	HCHO	wet chemical reduction	1 mol L^‒1 KOH	HER	40	[141]
B-Os aerogels	NaBH₄	wet chemical reduction	full pH range	HER	12, 19 and 33 respectively in 0.5 mol L^‒1 H₂SO₄, 1 mol L^‒1 KOH, and 1 mol L^‒1 PBS electrolyte	[129]
PdHx@Ru metallenes	HCHO	wet chemical reduction	1 mol L^‒1 KOH	HER	30	[165]
Pd@Pd-P@Pt sandwich nanocubes	TOP	wet chemical reduction	1 mol L^‒1 KOH	HER	MA = 5.02 A mg⁻¹_Pt@−0.07 V	[163]

Fig. 18. (a) Proposed electrocatalytic mechanisms of PtP NDs for HER, green: Pt; red: P; orange: O; and white: H. (b) Linear sweep voltammetry curves of PtP NDs, Pt NDs, and commercial Pt/C in 0.5 mol L-1 H2SO4 at a scan rate of 5 mV s-1. Reprinted with permission from Ref. [85]. Copyright 2022, Wiley-VCH.

Fig. 19. (a) Calculations of H and OH binding energies of B doped Pd (111) for the HOR plotted as a function of the calculated εd referenced to the Fermi energy. Reprinted with permission from Ref. [36]. Copyright 2022, Wiley-VCH. (b) The optimized structures of catalytic sites and electronic localization function for IrPd (111) and IrPdH (111) surface. Reprinted with permission from Ref. [49]. Copyright 2022, Wiley-VCH. (c) Creation of tunable lattice strain on Pt shells through the continuous volume expansion of Pd nanocubes tuning phosphorization degrees of Pd-P cores. (d) The correlation between normalized HER catalytic activities (the black line represents MA and the red line represents SA) of all strained Pt shells and strain of Pt shells. Reprinted with permission from Ref. [163]. Copyright 2021, Springer Nature.

Fig. 20. (a) The hydrogen adsorption free energy (ΔGH*) on Ru, P1-Ru, P2-Ru, and P3-Ru, respectively. (b) Reaction paths of P2-Ru and Ru toward alkaline HER and HOR. Reprinted with permission from Ref. [43]. Copyright 2022, American Chemical Society. (c) Calculated Gibbs free energies of *OH onto different locations of B-Ru (002) and Ru (002). (d) Two H* atoms on the Ru surface recombine to form H2, and *OH desorbs from the B sites of B doped Ru@CNT. Reprinted with permission from Ref. [76]. Copyright 2022, Elsevier.

Table 4 Summary of nonmetal doped PGM-based catalysts for liquid small molecule oxidation reactions.

Catalyst	Nonmetal source	Synthesis method	Electrolyte	Reaction	Performance	Ref.
P doped Pt Nanodendrites	NaH₂PO₂	wet chemical reduction	1.0 mol L^‒1 KOH + 1.0 mol L^‒1 methanol	MOR	MA = 4.2 A mg_Pt^-1	[85]
P-Doped Ag@Pd nanoparticles	triphenyl phosphorous	wet chemical reduction	1 mol L^‒1 KOH + 1 mol L^‒1 ethanol	EOR	MA = 7.2 A mg_Pd^-1	[43]
P-doped PtNi concave nanocubes	TOP	wet chemical reduction	0.5 mol L^‒1 H₂SO₄ + 2 mol L^‒1 CH₃OH	MOR	MA = 0.38 A mg_Pt^-1, SA = 3.85 mA cm^-2	[88]
PdBP NWs	NaH₂PO₂, DMAB, H₃BO₃	wet chemical reduction	1 mol L^‒1 KOH and 1 mol L^‒1 ethanol	EOR	MA = 4.15 A mg_Pd^-1	[64]
PdBP nanorods	NaH₂PO₂, NaBH₄	wet chemical reduction	0.5 mol L^‒1 H₂SO₄ +0.5 mol L^‒1 HCOOH	FAOR	MA = 1.32 A mg_Pd^-1, SA = 5.58 mA cm^-2	[89]
Pt-Ni-P nanocages	NaH₂PO₂	wet chemical reduction	0.5 mol L^‒1 H₂SO₄ and 1 mol L^‒1 CH₃OH	MOR	MA = 1.22 A mg_Pt^-1, SA = 2.28 mA cm^-2	[173]
PdH_0.43@Pt octahedral nanoparticles	DMF	wet chemical reduction	1.0 mol L^‒1 KOH +1.0 mol L^‒1 methanol	MOR	MA = 3.68 A mg^-1	[170]
Pd@Pd-P@Pt sandwich nanocubes	TOP	wet chemical reduction	0.5 mol L^‒1 H₂SO₄ and 1 mol L^‒1 CH₃OH	MOR	MA = 2.94 A mg^-1@0.65V, SA = 12.82 mA cm^-2@0.65V	[163]

Fig. 21. The mechanism for MOR/EOR/FAOR, light green: surface PGMs, dark green: nonmetal, black: poisoned PGMs.

Fig. 22. (a) In-situ Fourier transform infrared spectroscopy spectra of MOR on P-PtNi CNC. (b) MA and SA of P-PtNi CNC, PtNi CNC, commercial PtRu/C and commercial Pt/C in 0.5 mol L?1 H2SO4 and 2 mol L?1 CH3OH. Reprinted with permission from Ref. [88]. Copyright 2022, Springer Nature. (c) Scheme of the preparation. (d) Pt mass-normalized histogram. (e) Durability evaluation by chronoamperometry tests at 0.77 V vs. RHE. Reprinted with permission from Ref. [170]. Copyright 2021, American Chemical Society. (f) Free-energy diagrams for formic acid decomposition via the H-COO*, *COOH and OC-OH* pathways over Pd(111) and Pd(B/OSS)0.5 ML. Reprinted with permission from Ref. [172]. Copyright 2015, American Chemical Society.

Fig. 23. Future attractive research directions of nonmetal doped-PGMs catalysts.

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