Light alloying element-regulated noble metal catalysts for energy-related applications

doi:10.1016/S1872-2067(21)63899-8

Chinese Journal of Catalysis ›› 2022, Vol. 43 ›› Issue (3): 611-635.DOI: 10.1016/S1872-2067(21)63899-8

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Light alloying element-regulated noble metal catalysts for energy-related applications

Hui Chen^a, Bo Zhang^b, Xiao Liang^a, Xiaoxin Zou^a^,^*()

^aState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, Jilin, China
^bInternational Center of Future Science, Jilin University, Changchun 130012, Jilin, China

Received:2021-04-29 Revised:2021-04-29 Online:2022-03-18 Published:2022-02-18
Contact: Xiaoxin Zou
About author:Xiaoxin Zou has received his Ph.D. in inorganic chemistry from Jilin University (China) in June 2011; and then moved to the University of California, Riverside, and Rutgers, The State University of New Jersey, as a postdoctoral scholar from July 2011 to October 2013. He is currently a professor at the State Key Laboratory of Inorganic Synthesis and Preparative Chemistry in Jilin University. His research interests are in hydrogen energy materials chemistry, comprising the elucidation of the atomic basis for water-splitting electrocatalysts, the prediction and searching of efficient catalysts with novel crystal structures as well as the development of original catalyst design principles. Some of his recent progresses include the computation-driven structural design/engineering of water splitting catalysts, the structural understanding and synthetic methods of interstitial intermetallic catalysts, the design principles of low-iridium oxygen-evolution catalysts for PEM electrolyzers, and the synthetic strategies of large-area, highly stable electrode materials. He has authored 80+ peer-reviewed papers and 10 patents. He joined the editorial board of Chin. J. Catal. in 2020.
Supported by:
National Natural Science Foundation of China(21922507);National Natural Science Foundation of China(21771079);National Natural Science Foundation of China(21901083);National Natural Science Foundation of China(21621001);Jilin Province Science and Technology Development Plan(YDZJ202101ZYTS126);Fundamental Research Funds for the Central Universities(21901083);China Postdoctoral Science Foundation(2021M691202);111 Project(B17020)

Abstract

Abstract:

Noble metals have been widely used as heterogeneous catalysts because they exhibit high activity and selectivity for many reactions of both academic and industrial interest. The introduction of light atomic species (e.g., H, B, C, and N) into noble metal lattices plays an important role in optimizing catalytic performance by modulating structural and electronic properties. In this review, we present a general overview of the recent advances in the modification of noble metals with light alloying elements for various catalytic reactions, particularly for energy-related applications. We summarize the types, location, concentration, and ordering degree of light atoms as major factors in the performance of noble metal-based catalysts, with emphasis on how they can be rationally controlled to promote activity and selectivity. We then summarize the synthetic strategies developed to incorporate light elements and highlight the theoretical and experimental methods for understanding the alloying effects. We further focus on the wide usage of noble metal-based catalysts modified with different light alloying atoms and attempt to correlate the structural features with their catalytic performances. Finally, we discuss current challenges and future perspectives regarding the development of highly efficient noble metal-based catalysts modified with light elements.

Key words: Noble metal, Heterogeneous catalysis, Light element, Alloy, Electronic structure

Hui Chen, Bo Zhang, Xiao Liang, Xiaoxin Zou. Light alloying element-regulated noble metal catalysts for energy-related applications[J]. Chinese Journal of Catalysis, 2022, 43(3): 611-635.

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Figures/Tables 22

Fig. 1. Light elements and noble metal elements contained in this review for the construction of alloy catalysts; r, χ, and EC represent atomic radius, electronegativity, and electronic configuration, respectively.

Fig. 2. Stacking structures of pure Pd with fcc atomic arrangements (a), PdHx alloy comprising a disordered hydrogen distribution in fcc-Pd lattices (b), PdBx alloy comprising a disordered boron distribution in hcp-Pd lattices (c), Pd2B comprising an ordered boron distribution in hcp-Pd lattices (d). Note that fcc represents an a-b-c-a-b-c… stacking pattern, and hcp represents an a-b-a-b-… stacking pattern.

Fig. 3. Summary of the main functions of light alloying elements affecting catalytic activity, including phase transition (a), charge transfer (b), strain effect (c), ligand effect (d), ensemble effect (e), and subsurface chemistry (f).

Fig. 4. (a) Formation energies of RhX (X = B, C, and N), and integrated COHP values of Rh?X and X?X bonding; (b) Crystal structure of RhB; (c) Calculated free-energy diagrams of RhB, hcp-Rh, fcc-Rh, and Pt for HER at equilibrium potential. (a?c) Reproduced with permission [48]. Copyright 2021, Royal Society of Chemistry. (d) Pd d-band center and ΔGH* of Pd-B models in which interstitial B atoms vary from sub-surface to bulk; (e) Volcano plot displaying the ΔGH* values over Pd-B models with different concentrations of subsurface boron as a function of their surface Pd d-band centers; (f) Comparison of electrochemical active surface areas (ECSA) and ECSA-normalized specific activities for Pd2B, Pd, Pt, and two disordered B-doped Pd. (d?f) Reproduced with permission [30]. Copyright 2021, Elsevier.

Fig. 5. Summary of the main strategies for light element incorporation, including in-situ formation during catalysis (a), diffusion from the supports (b), wet chemical reduction (c), and high-temperature solid-state methods (d).

Fig. 6. (a) Schematic of hydrogen and carbon atoms dissolving in Pd catalysts and modifying the selectivity during alkyne hydrogenation. Reproduced with permission [14]. Copyright 2008, American Association for the Advancement of Science. (b) Schematic of boron diffusion from a porous BN support to a palladium subsurface. Reproduced with permission [66]. Copyright 2020, Wiley-VCH. (c) Schematic of the wet chemical synthesis of Pd-H nanostructures and lattice spacing changes from Pd to Pd-H. Reproduced with permission [33]. Copyright 2020, Chinese Chemical Society. (d) Selective synthesis of four phase-pure Ru-B intermetallics through solid state reactions. Reproduced with permission [99]. Copyright 2020, Royal Society of Chemistry.

Fig. 7. Schematic summarizing microscopy, diffraction, spectroscopy, and in situ techniques for characterization of alloy catalysts.

Fig. 8. (a) Schematic of the octahedral interstices (O sites) and tetrahedral interstices (T sites) in Pd hydride; dDPC (b) and iDPC (c) STEM images of PdHx. Reproduced with permission [67]. Copyright 2020, Wiley-VCH. (d) Schematic of the in situ EELS measurement on (e) a single Pd nanocrystal. (f,g) EEL spectra recorded on the Pd nanocrystal at varying H2 pressures. Reproduced with permission [108]. Copyright 2014, Nature Research.

Fig. 10. (a) Schematic of in situ ATR-SEIRAS in conjunction with DEMS, GC, and NMR analysis during Pd-catalyzed CO2RR; (b) Variation of CO coverages on Pd and Pd-B catalysts over potential. Reproduced with permission [32]. Copyright 2008, American Association for the Advancement of Science.

Fig. 11. Schematic of the main catalytic reactions studied using light element-modified noble metal systems (left: electrocatalysis; right: thermocatalysis).

Table 1 List of synthesis, structure, and catalytic application of some representative H-modified noble metal catalysts.

Catalyst	Synthesis method	H source	Structure	Reaction ^a	Ref.
PdH_0.4 nanocubes	two-step wet chemical method	DMF	fcc structure	CO₂RR	[122]
PdH_x nanoparticles	In-situ formation during catalysis	H₂	fcc structure (α+β phase)	CO₂RR	[62]
Pd-H icosahedra	eet chemical method	DMF	fcc structure	ORR	[33]
PdH_0.7 nanocubes	eet chemical method	DMF	fcc structure (β phase)	ORR	[72]
PdH_0.43 nanocrystals	solvothermal method	n-butylamine	fcc structure	FAOR	[70]
PdH_x nanocrystals	H absorption under CO/H₂ mixture	H₂	fcc structure (β phase)	FAOR	[139]
PdH cubes and octahedra nanocrystals	wet chemical method	DMF	fcc structure (β phase)	FAOR/MOR	[69]
PdH_0.43 nanocrystals	wet chemical method	DMF	fcc structure (β phase)	MOR	[68]
PdH_0.43 nanoparticles	solvothermal method	n-butylamine	fcc structure	COOR	[71]
Nanoporous PdH_0.43	solvothermal method	DMF	fcc structure	NRR	[123]
PdH_x nanoparticles	in situ formation during catalysis	H₂	fcc structure	HER	[61]
RhPdH bimetallene nanosheets	solvothermal method	formaldehyde	fcc structure (β phase)	HER	[34]
RhPd-H nanoparticles	solvothermal method	acetaldehyde	fcc structure	HER	[137]
MoPdH nanosheets	solvothermal method	oleylamine	fcc structure	MOR, EOR, EGOR	[136]

Fig. 12. Schematics of the synthetic route (a) and the proposed NRR pathway (b) for nanoporous PdH0.43. Reproduced with permission [123]. Copyright 2020, Wiley-VCH. (c) XRD and of PdH0.43 nanocrystals; (d) MOR catalytic properties of Pd and PdH0.43 nanocrystals. (b,c) Reproduced with permission [68]. Copyright 2015, American Chemical Society.

Fig. 13. (a) Calculated ΔGH* values at different sites on RhPd (111) and RhPd-H (111) surfaces; (b) Catalytic activity comparison of RhPd-H, RhPd, and reference catalysts. (a,b) Reproduced with permission [137]. Copyright 2019, American Chemical Society. (c) Schematic of the formation energy of 2D RhPd alloy and 2D RhPd alloy hydride; (d) TEM image of RhPd-H bimetallene nanosheets. (c,d) Reproduced with permission [34]. Copyright 2020, American Chemical Society.

Table 2 List of structure, synthesis, and catalytic application of some representative B-modified noble metal catalysts.

Catalyst	Synthesis method	B source	Structure	Reaction	Ref.
B-doped Pd nanoparticles	wet chemical reduction	BH₃,THF	fcc structure	alkyne hydrogenation	[77]
Porous BN supported Pd	impregnation	BN	fcc structure	alkyne hydrogenation	[66]
Mesoporous Pd₂B nanoparticles	wet chemical method	DMAB	hcp and fcc structure	p-nitrophenol reduction	[49]
Pd-B films	electrochemical deposition	DMAB	fcc structure	CO₂RR	[32]
B-doped Pd nanoparticles	wet chemical method	Boric acid	fcc structure	formate oxidation	[79]
PdCuB nanoparticles	wet chemical method	DMAB	fcc structure	EOR	[73]
Mesoporous Pd-B nanospheres	wet chemical method	DMAB	fcc structure	EOR	[147]
RuB	metallothermic reduction	MgB₂	Hexagonal structure	HER	[53]
RuB₂	solid-state metathesis	MgB₂	Orthorhombic structure	HER	[98,99]
RhB	solid-phase reaction	MgB₂	hcp structure	HER	[48]
Pd₂B	solid-phase reaction	MgB₂	hcp structure	HER	[30]
Rh-Ni-B nanoparticles	wet chemical method	NaBH₄	fcc structure	hydrous hydrazine decomposition	[76]
B-doped Pd nanoparticles	wet chemical method	NaBH₄, DMAB	fcc structure	gormic acid decomposition	[142,143]
B-doped Pd nanoparticles	wet chemical method	DMAB	fcc structure	ORR	[31,75,145]

Fig. 14. (a) Schematic of the synthesis; (b) TEM image of mesoporous Pd-B alloy nanospheres. (a,b) Reproduced with permission [147]. Copyright 2019, Royal Society of Chemistry. SEM (c), TEM and high-resolution TEM (d) of images of hcp-mesoPd2B. (c,d) Reproduced with permission [49]. Copyright 2020, American Chemical Society.

Fig. 15. (a) Schematic of the effect of metal-boron orbital interaction on hydrogen adsorption for metal-boron intermetallics; (b) A volcano plot exhibiting the exchange current densities as a function of ΔGH* values for different HER catalysts. (a,b) Reproduced with permission [53]. Copyright 2020, Wiley-VCH. (c) Crystal structures of RuB2; (d) Fitted linear relationship between the ΔGH* values and the metal d-band center for MB2, Pt, and Ru; (e) HER polarization curves for RuB2 and Pt/C in alkaline electrolyte. (c?e) Reproduced with permission [98]. Copyright 2019, Wiley-VCH.

Fig. 16. SEM (a) and TEM (d) images of C-Au catalysts supported on ordered mesoporous carbon; (c) Energy profiles for H2 dissociation at Au and C-Au surfaces. (a?c) Reproduced with permission [80]. Copyright 2020, Nature Research. Bright-field (BF)-STEM (d) and ABF-STEM (e) images of Rh2C. The inset of (e) shows the structural model of Rh2C. (f) ΔGH* values for HER of Rh2C, Rh, and Pd, respectively. (d?f) Reproduced with permission [81]. Copyright 2020, American Chemical Society.

Fig. 17. (a) Schematics of structural-dependent selectivity for NH3 catalytic oxidation over supported Pd nanoparticles. The Pd, N, H, and O atoms are in green, blue, white and red, respectively. (b) In situ Pd L3-edge XANES spectra of supported Pd catalysts in different gas environments. (c) Catalytic behavior of supported Pd catalysts for NH3 oxidation at increasing temperatures. Reproduced with permission [15]. Copyright 2019, Nature Publishing Group.

Fig. 18. (a) Schematic of the synthesis of Pd3S; (b) Structural resemblance of Pd3S (left) and Pd4S (right) surfaces; (c) Catalytic activity for alkyne semi-hydrogenation as a function of the differential adsorption energy of acetylene and ethene for Pd3S, Pd4S, and reference catalysts. (a?c) Reproduced with permission [54]. Copyright 2018, Nature Publishing Group. (d) TEM image of AgP2 nanocrystals; (e) Schematic of the selective CO2-to-syngas reaction on AgP2. (d,e) Reproduced with permission [50]. Copyright 2019, Nature Publishing Group.

Fig. 19. (a) Schematic of the interstitial Si incorporation strategy for promoting Ru top site from subordinate to dominant status; (b) HER polarization curves of RuSi, Ru, Pt, and Si in acidic electrolyte. Reproduced with permission [55]. Copyright 2019, Wiley-VCH. (c) Proposed catalytic activation pathway for ammonia synthesis over LaRuSi; (d) Catalytic performances for ammonia synthesis over LaRuSi, CaRuSi, and LaRu2Si2. Reproduced with permission [94]. Copyright 2019, Wiley-VCH.

Fig. 20. Future research directions of light element-modified metal systems in heterogeneous catalysis.

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Light alloying element-regulated noble metal catalysts for energy-related applications

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