高熵纳米合金在电化学催化中的应用

doi:10.3866/PKU.WHXB202009077

Abstract

Abstract:

The implementation of clean energy techniques, including clean hydrogen generation, use of solar-driven photovoltaic hybrid systems, photochemical heat generation as well as thermoelectric conversion, is crucial for the sustainable development of our society. Among these promising techniques, electrocatalysis has received significant attention for its ability to facilitate clean energy conversion because it promotes a higher rate of reaction and efficiency for the associated chemical transformations. Noble-metal-based electrocatalysts typically show high activity for electrochemical conversion processes. However, their scarcity and high cost limit their applications in electrocatalytic devices. To overcome this limitation, binary catalysts prepared by alloying with transition metals can be used. However, optimization of the activity of the binary catalysts is considerably limited because of the presence of the miscibility gap in the phase diagram of binary alloys. The activity of binary electrocatalysts can be attributed to the adsorption energy of molecules and intermediates on the surface. High-entropy alloys (HEAs), which consist of diverse elements in a single NP, typically exhibit better physical and/or chemical properties than their single-element counterparts, because of their tunable composition and inherent surface complexity. Further, HEAs can improve the performance of binary electrocatalysts because they exhibit a near-continuous distribution of adsorption energy. Recently, HEAs have gained considerable attention for their application in electrocatalytic reactions. This review summarizes recent research advances in HEA nanostructures and their application in the field of electrocatalysis. First, we introduce the concept, structure, and four core effects of HEAs. We believe that this part will provide the basic information about HEAs. Next, we discuss the reported top-down and bottom-up synthesis strategies, emphasizing on the carbothermal shock method, nanodroplet-mediated electrodeposition, fast moving bed pyrolysis, polyol process, and dealloying. Other methods such as combinatorial co-sputtering, ultrashort-pulsed laser ablation, ultrasonication-assisted wet chemistry, and scanning-probe block copolymer lithography are also highlighted. Among these methods, wet chemistry has been reported to be effective for the formation of nano-scale HEAs because it facilitates the concurrent reduction of all metal precursors to form solid-solution alloys. Next, we present the theoretical investigation of HEA nanocatalysts, including their thermodynamics, kinetic stability, and adsorption energy tuning for optimizing their catalytic activity and selectivity. To elucidate the structure–property relationship in HEAs, we summarize the research progress related to electrocatalytic reactions promoted by HEA nanocatalysts, including the oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, methanol oxidation reaction, and CO₂ reduction reaction. Finally, we discuss the challenges and various strategies toward the development of HEAs.

Key words: High-entropy alloy nanostructures, Electrocatalysis, Single-phase solid solution, Adsorption energy, Active site

Kangning Zhao, Xiao Li, Dong Su. High-Entropy Alloy Nanocatalysts for Electrocatalysis[J]. Acta Phys. -Chim. Sin. 2021, 37(7), 2009077. doi: 10.3866/PKU.WHXB202009077

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Composition	Synthetic method	Structure	Catalytic application	Ref.
RuRhCoNi(Ir)	Carbothermal shock	FCC	NH₃ decomposition	36
RuRhCoNiIr	Wet impregnation	Phase separation	NH₃ decomposition	36
FeCoNiCuMo	Carbothermal shock	FCC	NH₃ decomposition	35
PtPdRhRuCe	Carbothermal shock	FCC	NH₃ oxidation	37
PtPdRhCoCe	Carbothermal shock	FCC	NH₃ oxidation	37
PtPdRhNi	Carbothermal shock	FCC	ORR ^a	45
PtPdFeCoNi	Carbothermal shock	FCC	ORR	45
PtRuCuOsIr	Mechanical alloying & dealloying	FCC	ORR, MOR ^b	38
PdAuAgTi	–	–	ORR	39
CrMnFeCoNi,	Combinatorial co-sputtering	–	ORR	41
AlNiCoIrMo	Arc-melting & dealloying	FCC	ORR	44
AlNiCuPtM (M = Ir, Pd, V, Co, Mn)	Arc-melting & dealloying	FCC	ORR	40
AlNiCuPtPdAu	Arc-melting & dealloying	FCC	HER ^c, OER ^d	43
CoCrFeMnNi	Kinetically-controlled laser-synthesis	FCC	HER	49
PtAuPd(RhRu)	Ultrasonication-assisted wet chemistry	FCC	HER	48
CoFeLaNiPt	Nanodroplet-mediated electrodeposition	Amorphous	HER, OER	47
FeNiMnCrCu	Arc-melting	FCC + BCC	OER	50
MnFeCoNi	Mechanical alloying	FCC	OER	51
AlNiCoFeM (M = Mo, Nb, Cr)	Arc-melting & dealloying	FCC	OER	53
MnFeCoNiCu	MOF-template method	FCC	OER	52
PtFeCoNiCuAg	Radio frequency sputter depositions	FCC	MOR	55
IrOsPtRhRu	Thermal decomposition	FCC/HCP	MOR	56
CuAgAuPtPd	Arc-melting & mechanical alloying	FCC	MOR	57
AgAuCuPdPt	Melting & cryogrinding	FCC	CO₂RR ^e	16

Reaction	Composition	Structural feature	E_1/2/V_RHE	Tafel slope/(mV∙dec⁻¹)	Electrolyte	Ref.
ORR	PtPdRhNi	Nanoparticles	0.86	32	1.0 mol∙L⁻¹ KOH	45
	PtPdFeCoNi	Nanoparticles	0.85	31	1.0 mol∙L⁻¹ KOH	45
	PtRuCuOsIr	Nanoporous	0.864	–	0.1 mol∙L⁻¹ HClO₄	38
	CrMnFeCoNi,	Nanoparticles	–	82 ± 12	3 mol∙L⁻¹ KCl	41
	AlNiCuPtPdAu	Nanoporous	0.9	–	0.1 mol∙L⁻¹ HClO₄	44
	AlNiCuPtMn	Nanoporous	0.945	47	0.1 mol∙L⁻¹ HClO₄	40
Reaction	Composition	Structural feature	Overpotential/mV	Tafel slope/(mV·dec⁻¹)	Electrolyte	Ref.
HER	AlNiCuPtPdAu	Nanoporous	–	28	0.1 mol∙L⁻¹ HClO₄	43
	AlNiCoIrMo	Nanoporous	18.5	33.2	0.5 mol∙L⁻¹ H₂SO₄	44
	PtAuPd(RhRu)	Nanoparticles	90	62	1.0 mol∙L⁻¹ KOH	48
	CoFeLaNiPt	Nanoparticles	555		0.1 mol∙L⁻¹ KOH	47
Reaction	Composition	Structural feature	Overpotential/mV	Tafel slope/(mV·dec⁻¹)	Electrolyte	Ref.
OER	CoFeLaNiPt	Nanoparticles	377	–	0.1 mol∙L⁻¹ KOH	47
	FeNiMnCrCu	-	342	58	1 mol∙L⁻¹ NaOH	50
	MnFeCoNi	Nanoporous	302	83.7	1 mol∙L⁻¹ KOH	51
	AlNiCoFeMo	Nanoporous	240	46	1 mol∙L⁻¹ KOH	53
	MnFeCoNiCu	Nanoparticles	263	43	1.0 mol∙L⁻¹ KOH	52
Reaction	Composition	Structural feature	I_f/I_b	Mass activity/(mA∙mg_Pt⁻¹)	Electrolyte	Ref.
MOR	PtFeCoNiCuAg	Nanoparticles	1.09	0.504	0.5 mol∙L⁻¹ H₂SO₄ 1.0 mol∙L⁻¹ CH₃OH	55
MOR	IrOsPtRhRu	Nanoporous	1.26	0.86	0.5 mol∙L⁻¹ H₂SO₄ 0.5 mol∙L⁻¹ CH₃OH	38

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High-Entropy Alloy Nanocatalysts for Electrocatalysis

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