Rational design and precise manipulation of nano-catalysts

doi:10.1016/S1872-2067(21)63933-5

Abstract

Abstract:

Nano-catalysis plays a vital role in the chemical transformations and significantly impacts the booming modern chemical industry. The rapid technological enhancements have resulted in serious energy and environmental issues, which are currently spurring the exploration of the novel nano-catalysts in diverse fields. In order to develop the efficient nano-catalysts, it is essential to understand their fundamental physicochemical properties, including the coordination structures of the active centers and substrate-adsorbate interactions. Subsequently, the nano-catalyst design with precise manipulation at the atomic level can be attained. In this account, we have summarized our extensive investigation of the factors impacting nano-catalysis, along with the synthetic strategies developed to prepare the nano-catalysts for applications in electrocatalysis, photocatalysis and thermocatalysis. Finally, a brief conclusion and future research directions on nano-catalysis have also been presented.

Key words: Nano-catalysis, Single-atom catalysts, Water splitting, Oxygen reduction reaction, CO₂ reduction reaction, Silane oxidation, Benzene oxidation, N-formylation

Qinggang Liu, Junguo Ma, Chen Chen. Rational design and precise manipulation of nano-catalysts[J]. Chinese Journal of Catalysis, 2022, 43(4): 898-912.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63933-5

https://www.cjcatal.com/EN/Y2022/V43/I4/898

Figures/Tables 11

Fig. 1. Overview of the topics covered in this account.

Fig. 2. (a) Schematic illustration of the preparation for the CoP/NCNHP; (b) The linear sweep voltammetry (LSV) curve of the CoP/NCNHP// CoP/NCNHP electrode in 1 mol/L KOH with iR compensation in a two-electrode system; (c) Chronopotentiometric curve of water electrolysis at different current densities in 1 mol/L KOH; (d) Calculated density of states (DOS) for CoP/NCNHP and pure CoP; (e) Charge density distribution maps of the CoP/NCNHP catalyst; (f) Calculated free energy diagram of the HER on CoP, surface-oxidized 50% CoP, and surface-oxidized 100% CoP, respectively. Reprinted with permission from Ref. [73]. Copyright 2018, American Chemical Society.

Fig. 3. (a) LSV curves of MoP@NCHSs-T, bulk MoP, and commercial 20% Pt/C in 1.0 mol/L KOH; (b) Stability of the MoP@NCHSs-900 catalyst in 1.0 mol/L KOH; (c) Average Bader charge of N-doping carbon; (d) Free energy diagram of the water dissociation step. Reprinted with permission from Ref. [74]. Copyright 2019, John Wiley and Sons.

Fig. 4. (a) Schematic illustrations and corresponding TEM images of the samples during the evolution process from polyhedral to nanoframes; (b) HAADF-STEM image and corresponding EDX data (mapping and line-scan) of annealed hollow Pt3Ni nanoframe; (c) Specific activities measured at 0.95 V, and improvement factors versus Pt/C catalysts; (d) ORR polarization curves and corresponding Tafel plots (inset) of Pt3Ni frames before and after 10000 potential cycles. Reprinted with permission from Ref. [80]. Copyright 2014, American Association for the Advancement of Science.

Fig. 5. (a) Schematic illustration of the preparation for the Co-N5/HNPCSs catalyst; (b) HAADF-STEM and EDS images of the Co-N5/HNPCSs catalyst; LSV curves (c) and FECO and FEH2 (d) of the Co-N5/HNPCSs and CoPc catalysts; (e) Calculated free energy of CO2RR. Reprinted with permission from Ref. [82]. Copyright 2018, American Chemical Society.

Fig. 6. (a) Current-voltage curves for different samples from LSV scans; (b) FECO and FEH2 of different Cu-loaded samples at -0.78 V (vs. RHE); (c) Free energy profiles for CO2 activation on Cu, Cu@Cu2O and Cu-APC. (d) Configurations of physisorbed CO2 and chemisorbed CO2 on Cu-APC. Reprinted with permission from Ref. [83]. Copyright 2019, Springer Nature.

Fig. 7. (a) Schematic illustration of photoinduced hole on {110} and {001} of WO3 during BA oxidation. (b) Morphology model and HRTEM graph of WO3 nanowire and nanosheet. Dynamics of carriers on two crystal facets: hole mobility (c); electron mobility (d); hole diffusion length (e); reaction rates of benzyl alcohol oxidation (f); steady state fluorescence (g); and hole lifetime (h). Reprinted with permission from Ref. [90]. Copyright 2018, American Chemical Society.

Fig. 8. (a) Schematic illustration of the structure and catalytic mechanism of p-BWO; (b) TEM image of the p-BWO nanosheets; (c) Digital photographs of p-BWO in the initial versus coloured state; (d) Photoluminescence emission spectra (excitation at 340 nm) of the p-BWO and pristine Bi2WO6; (e) Conversion rate of toluene oxidation for Bi2WO6 and p-BWO with different substrate loadings; (f) Schematic of the separation of photoinduced carriers of p-BWO, and the mechanism of photocatalytic reaction and photochromism. Reprinted with permission from Ref. [93]. Copyright 2019, Springer Nature.

Fig. 9. (a) The aberration-corrected HAADF-STEM images of Au1/mpg-C3N4; (b) Fourier transform magnitudes of the EXAFS spectra for Au1/mpg-C3N4, Au NPs/mpg-C3N4 and Au foil; (c) Conversion rate of the diphenylmethylsilane in water with different Au catalysts; (d) The mechanism of silane oxidation over single-site Au catalyst. Reprinted with permission from Ref. [99]. Copyright 2018, John Wiley and Sons.

Fig. 10. The aberration-corrected HAADF-STEM images of the Fe-N4 SAs/N-C (a), Fe-N3C1 SAs/N-C (b), FeN2C2 SAs/N-C (c) catalysts. The insets are the corresponding structure model. (d) HAADF-STEM-EDS mapping of the Fe-N4 SAs/N-C catalyst; XANES spectra at the C K-edge (e), N K-edge (f), and Fe L-edge (g). Reprinted with permission from Ref. [103]. Copyright 2019, Springer Nature.

Fig. 11. (a) Illustration of the self-reduction method for the preparation of Pt1/Ti3-xC2Ty; (b) HAADF-STEM image of Pt1/Ti3-xC2Ty and corresponding intensity maps obtained in line 1 in (b); (c) Catalytic performance of the N-formylation of aniline using different catalysts and the recycling test of Pt1/Ti3-xC2Ty; (d) EXAFS spectra of Pt1/Ti3-xC2Ty; (e) Charge density difference of Pt1/Ti3-xC2Ty with a plain view. Reprinted with permission from Ref. [107]. Copyright 2019, American Chemical Society.

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