Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization

doi:10.1007/s40820-024-01347-y

Abstract

Abstract:

The exploration of sustainable energy utilization requires the implementation of advanced electrochemical devices for efficient energy conversion and storage, which are enabled by the usage of cost-effective, high-performance electrocatalysts. Currently, heterogeneous atomically dispersed catalysts are considered as potential candidates for a wide range of applications. Compared to conventional catalysts, atomically dispersed metal atoms in carbon-based catalysts have more unsaturated coordination sites, quantum size effect, and strong metal-support interactions, resulting in exceptional catalytic activity. Of these, dual-atomic catalysts (DACs) have attracted extensive attention due to the additional synergistic effect between two adjacent metal atoms. DACs have the advantages of full active site exposure, high selectivity, theoretical 100% atom utilization, and the ability to break the scaling relationship of adsorption free energy on active sites. In this review, we summarize recent research advancement of DACs, which includes (1) the comprehensive understanding of the synergy between atomic pairs; (2) the synthesis of DACs; (3) characterization methods, especially aberration-corrected scanning transmission electron microscopy and synchrotron spectroscopy; and (4) electrochemical energy-related applications. The last part focuses on great potential for the electrochemical catalysis of energy-related small molecules, such as oxygen reduction reaction, CO₂ reduction reaction, hydrogen evolution reaction, and N₂ reduction reaction. The future research challenges and opportunities are also raised in prospective section.

Key words: Dual-atom catalysts, Synergetic effect, Electrocatalysis, Oxygen reduction reaction, CO₂ reduction reaction, Hydrogen evolution reaction, N₂ reduction reaction

Yizhe Li, Yajie Li, Hao Sun, Liyao Gao, Xiangrong Jin, Yaping Li, Zhi LV, Lijun Xu, Wen Liu, Xiaoming Sun. Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization[J]. Nano-Micro Letters, 2024, 16(1): 139-.

Yizhe Li, Yajie Li, Hao Sun, Liyao Gao, Xiangrong Jin, Yaping Li, Zhi LV, Lijun Xu, Wen Liu, Xiaoming Sun. [J]. Nano-Micro Letters, 2024, 16(1): 139-.

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Figures/Tables 20

Fig. 1 a Advantages of dual-atom catalysts over single-atom catalysts. b-d Schematic diagram of the classification of DACs. The green ball and the orange ball represent the metal atoms M and M’, respectively. The white ball represents N or O atom. The blue cube represents the substrate

Fig. 2 a Schematic of Fe-N₄/Pt-N₄@NC [42]. Copyright 2021 Wiley-VCH GmbH. b Structure of FeCoN₆ [46]. Copyright 2023 Springer Nature. c Structural models of FeNi-N₆ (type I) and d FeNi-N₆ (type II) [48]. Copyright 2020 American Chemical Society

Fig. 3 a Free energy diagram for ORR on a single Fe site of molecular FePc. b Free energy diagram for ORR on two adjacent Fe sites of FePc nanorods [63]. Copyright 2022 American Chemical Society. c Partial density of state (pDOS) of Fe 3d orbitals. d Charge density difference. e pDOS for Fe-3d_yz/d_z²/d_xz orbitals and adsorbed CO orbitals. f Orbital interaction between Fe-3d (d_z² and d_xz/d_yz) and adsorbed CO (5σ and 2π*) [30]. Copyright 2022 American Chemical Society. g Least-squares curve-fitting analysis of operando EXAFS spectra at the Ni K-edge. h Comparison between the Ni K-edge XANES experimental spectra (solid lines) and the theoretical spectra (dashed lines) calculated with the depicted structures (insert). i Free energy diagrams for CO₂ electroreduction to CO. j Calculated Gibbs free energy diagrams for the HER and CO₂ electroreduction to HCOOH on O − Ni₂ − N₆. k Proposed reaction pathways on O − Ni₂ − N₆ [37]. Copyright 2022 American Chemical Society

Fig. 4 a ORR theoretical overpotential (η^ORR) versus ΔG_*OOH. b Volcano plots of the OER theoretical overpotential (η^OER) versus adsorption free energy difference (ΔG_*OOH—ΔG_*O). c Number of electrons (N_e) lost from an Fe, Co, or Ni atom [81]. Copyright 2022 American Chemical Society. d Density of states of Fe 3d for Fe-SAC and NiFe-DASC, of Ni 3d for Ni-SAC and NiFe-DASC. e Schematic illustration of orbital interactions between adsorbed CO (5σ and 2π*) and 3d orbital (d_z², d_xz/d_yz) of Fe site in e Fe-SAC and f NiFe-DASC [83]. Copyright 2021 Springer Nature

Fig. 5 Schematic electronic structures of a Fe-N-C and b Fe/Zn-N-C [88]. Copyright 2022 Royal Society of Chemistry. c Comparison of magnetic moment and ΔG_OH*. d Fe 3d DOS of Fe₁/Fe₁-2 and Cu₁/Fe₁-2. e DOS of the five Fe 3d orbitals in Cu₁/Fe₁-2 [89]. Copyright 2022 Wiley-VCH GmbH. f Geometric structure and corresponding electron density difference of Fe-Ni-N-P-C. g Overpotential of OOH* formation [91]. Copyright 2021 Elsevier Ltd

Fig. 6 a Schematic illustration for the two-step synthesis of Fe₂-N-C [93]. Copyright 2019 Elsevier Ltd. b Heteroatom modulator approach for fabricating dual-atom iron catalysts on carbon layer [95]. Copyright 2020 Wiley-VCH GmbH

Fig. 10 a Schematic diagram of the dual-solvent route for Fe-NiNC catalysts [105]. Copyright 2020 Elsevier Ltd. b Schematic illustration of A-CoPt-NC [106]. Copyright 2018 American Chemical Society

Fig. 11 a HAADF-STEM image of Cu/Ni-NC. b Line-scanning intensity profiles corresponding to the highlights in a. c EELS diagram of Cu/Ni-NC [47]. Copyright 2023 Wiley-VCH GmbH. d HAADF-STEM image of NiCu-NC. e NiCu atomic pair and the corresponding 3D intensity profile. f EELS diagram of NiCu-NC [108]. Copyright 2023 Wiley-VCH GmbH

Fig. 12 a Fe K-edge XANES spectra. b EXAFS fitting curve of Fe in Fe-Co DACs spectra. c k-space experimental EXAFS spectra and fitting curves of Fe in Fe-Co DACs [46]. Copyright 2023 Springer Nature. d Fe K-edge XANES spectra. e FT-EXAFS spectra. f Corresponding fitting in R space of FeCo-NSC and FePc at Fe K-edge [43]. Copyright 2022 Elsevier Ltd

Fig. 13 a Pt L₃-edge and b Fe K-edge FT-EXAFS spectra and the corresponding fitting curves under different potentials. c The fitting results of the coordination number. In situ SR-FTIR characterizations for d Pt = N₂ = Fe ABA and e Pt AMS. f FTIR absorption stretching for Pt = N₂ = Fe ABA and Pt AMS [40]. Copyright 2022 Springer Nature

Fig. 14 a The optimized structure model, b aberration-corrected HAADF-STEM image, c ⁵⁷Fe Mossbauer spectrum. d magnetic susceptibility of Fe,Mn/N-C. e LSV curves of Fe,Mn/N-C, Fe/N-C, Mn/N-C and Pt/C catalyst in 0.1 M HClO₄ solution [132]. Copyright 2021 Springer Nature. f Structure model, g HAADF-STEM image of FeCo-NC. h SCV measurements, i Tafel plots of the as-prepared catalysts 0.1 M KOH solution [128]. Copyright 2022 American Chemical Society

Table 1 The activity of DACs for ORR and their performance in different applications

Catalyst	E1/2 (V vs. RHE)	Electrolyte	Application	Peak power density (mW cm⁻²)	Refs
Fe-Se/NC	0.925	0.1 M KOH	Zn-air batteries	135	[137]
FeCo-NSC	0.86	0.1 M KOH	Zn-air batteries	152.8	[43]
FeCo-NC	0.877	0.1 M KOH	Zn-air batteries	372	[128]
CoFe-NG	0.952	0.1 M KOH	Zn-air batteries	230	[138]
Fe,Zn-N-C	0.867	0.1 M KOH	Zn-air batteries	138	[139]
Fe2DAC	0.898	0.1 M KOH	Zn-air batteries	325.8	[140]
D-FeCo-DAs-N-C	0.927	0.1 M KOH	Zn-air batteries	259	[141]
FeCo/DA@NC	0.84	0.1 M KOH	Zn-air batteries	110.3	[142]
Cu-Co/NC	0.92	0.1 M KOH	Zn-air batteries	295.9	[143]
Zn/Fe-NC	0.875	0.1 M KOH	Zn-air batteries	186.2	[144]
Fe-Mn-N-C	0.93	0.1 M KOH	AEMFCs	1321	[36]
FeCu-NC	0.882	0.1 M KOH	AEMFCs	910	[145]
FeCo-MHs	0.95	0.1 M KOH	AEMFCs	604.9	[146]
Fe-Mn-N-C	0.79	0.1 M HClO₄	PEMFCs*	1048	[36]
Fe, Cu DAs-NC	0.80	0.5 M H₂SO₄	PEMFCs	875	[147]
Fe&Pd-C/N	0.808	0.5 m H₂SO₄	PEMFCs	362	[148]
Cu-Co/NC	0.85	0.5 m H₂SO₄	PEMFCs	963	[143]
FeMo-N-C	0.84	0.1 M HClO₄	PEMFCs	460	[149]
FeCe-SAD/HPNC	0.81	0.1 M HClO₄	PEMFCs	771	[150]
(Au-Co) DP-NPAs	0.82	0.1 M HClO₄	PEMFCs	490	[84]

Fig. 15 a Illustration and b HAADF-STEM image of CoCu-DASC. c Line-scanning intensity profiles obtained from the site A and B in panel b. d Faradaic efficiencies for electrochemical reduction of CO₂ to CO, e CO partial current density in flow cell and f free energy profiles of CoCu-DASC and corresponding SACs [161]. Copyright 2022 Wiley-VCH GmbH g Illustration, h LSV curves, i Faraday efficiencies for electrochemical reduction of CO₂ to CO and j free energy profiles of Ni₂ DACs and Ni SAC [162]. Copyright 2022 Wiley-VCH GmbH

Fig. 16 a Schematic diagram of Pt-Ru dimers on NCNT. b HAADF-STEM images of Pt-Ru dimers. c K²-weighted magnitude of Fourier transform spectra of Pt-Ru dimers and Pt single atoms. d HER polarization curves and e normalized mass activity of Pt-Ru dimers and Pt single atoms at 0.05 V [171]. Copyright 2019 Springer Nature f DFT calculations of formation energies and d-band centre for bimetallic single-atom dimers. g HAADF-STEM image of NiCo-SAD-NC. h Ni K-edge and i Co K-edge FT-EXAFS spectra. j LSV curves and k corresponding Tafel plots [172]. Copyright 2021 Springer Nature

Fig. 17 a Illustration of FeM-GDYs. b Volcano relationship between the U_L and E_ads(*NH₂). c Colour contour plot of ΔG(*NNH) and ΔG(*NH₂) [181]. Copyright 2021 Royal Society of Chemistry. d HAADF-STEM image of PdCu/NC. e NH₃ yield rates and f FEs of Pd/NC, Cu/NC and PdCu/ NC [184]. Copyright 2021 Wiley-VCH GmbH

Fig. 18 a HAADF-STEM images of Co/Fe-SNC800. b Illustration of Co/Fe dual-metal site. c LSV curves of Fe-SNC800, Co-SNC800, Co/Fe-SNC800 at 1600 rpm. d Chronopotentiometry plots of Co/Fe-SNC800. e Reaction energy diagram of Co/Fe-SNC and Co-SNC under U = 0 V [196]. Copyright 2023 Royal Society of Chemistry. f Illustration of a-NiCo/NC. g LSV curves of a-NiCo/NC, NiCo NPs/NC, a-Ni/NC, a-Co/NC, RuO₂ at 1600 rpm. h Chronopotentiometry plots of a-NiCo/NC, NiCo NPs/NC, RuO₂. i Free energy diagram of a-NiCo/NC, a-Ni/NC, a-Co/NC under U = 0 V [85]. Copyright 2022 Wiley-VCH GmbH

Fig. 19 a Schematic synthesis of NiCu₃-N-C DAC. b LSV curves in 1 M NaOH + 0.2 M NH₄Cl. c N₂ selectivity of NiCu₃-N-C DAC in different initial concentrations of ammonia. Copyright 2023 Elsevier Ltd. d Preferable configuration of two metal atoms anchored C₂N (C, grey; N, blue; gold, M¹; pink, M²). e Reaction pathways based on the TER mechanism. f d-band centres and the adsorption energies of CO, O₂, and O for the Fe₂@C₂N, Fe₁Cu₁@C₂N and Cu₂@C₂N [209]. Copyright 2019 Wiley-VCH GmbH

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