Coordination environment of active sites and their effect on catalytic performance of heterogeneous catalysts

doi:10.1016/S1872-2067(21)63924-4

Chinese Journal of Catalysis ›› 2022, Vol. 43 ›› Issue (4): 928-955.DOI: 10.1016/S1872-2067(21)63924-4

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Coordination environment of active sites and their effect on catalytic performance of heterogeneous catalysts

Chunpeng Wang^a^,^†, Zhe Wang^b^,^c^,^†, Shanjun Mao^a^,^c, Zhirong Chen^b^,^c, Yong Wang^a^,^c^,^*()

^aAdvanced Materials and Catalysis Group, Institute of Catalysis, Zhejiang University, Hangzhou 310028, Zhejiang, China
^bCollege of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310028, Zhejiang, China
^cCenter of Chemistry for Frontier Technologies, Zhejiang University, Hangzhou 310028, Zhejiang, China

Received:2021-07-18 Accepted:2021-07-18 Online:2022-03-05 Published:2022-03-01
Contact: Yong Wang
About author:Yong Wang received his BS degree from Xiangtan University and his PhD degree from Zhejiang University. After a postdoctoral stay at the Department of Chemistry, Zhejiang University, he joined the Max Planck Institute for Colloids and Interfaces in Potsdam/Germany in 2009. He rejoined Zhejiang University and became a professor for Chemistry in 2011. Now he is Ph.D. supervisor, director of the Institute of Catalysis at the Department of Chemistry in Zhejiang University. He was included in the Highly Cited Researcher list by Clarivate Analytics 2020 and 2021 (Web of Science™, Thomson Reuters) in the field of Cross-Field and Chemistry, respectively. His research group has been focusing on the basic science and applied research for the design and development of novel materials for heterogeneous catalysis and energy conversion. The group strives to pursue green energy technologies and the fundamental science that make these technologies a reality. He joined the Editorial Board of Chin. J. Catal. in 2020.
First author contact:
^†Contributed to this work equally.
Supported by:
National Natural Science Foundation of China(21872121);National Natural Science Foundation of China(21908189);Key R&D Project of Zhejiang Province(2020C01133)

Abstract

Abstract:

The structural complexity of supported metal catalysts, playing significant role in a wide range of chemical technologies, have prevented us from deeply understanding their catalytic mechanisms at atomic level. A fundamental understanding of the nature of active sites and structure-performance relationship of supported metal catalysts from a comprehensive view will open up numerous new opportunities for the development of advanced catalysts to address the global challenges in energy conversion and environmental protection. This review surveys the effects of multiple factors, including the metal size, shape, support, alloy and ligand modifier, on the coordinated environment of active center and further their influence on the catalytic reactions, aiming to provide guidance for the design of industrialized heterogeneous catalysts with extraordinary performance. Subsequently, the key structure characterization techniques in determining the coordination structure of active metal sites, especially the dynamic coordination structure change under the reaction condition, are well summarized. A brief summary is finally provided together with personal perspectives on the further development in the field of heterogeneous metal catalysts.

Key words: Heterogeneous catalysis, Supported catalyst, Coordination environment, Metal catalyst, In-situ characterization

Chunpeng Wang, Zhe Wang, Shanjun Mao, Zhirong Chen, Yong Wang. Coordination environment of active sites and their effect on catalytic performance of heterogeneous catalysts[J]. Chinese Journal of Catalysis, 2022, 43(4): 928-955.

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Figures/Tables 18

Fig. 1. Brief summary of key impactors in manipulating local coordination environments of metal sites over the supported catalyst.

Fig. 2. (a) Fraction of surface atoms in uniform truncated octahedron nanoparticles a function of Au particle size. Reproduced with permission from Ref. [20]. Copyright 2007 Elsevier. (b) Relationship between the activity of CO oxidation at 300 K and the average size of the Au clusters supported over TiO2. Reproduced with permission from Ref. [40]. Copyright 1998, Science AAAS.

Fig. 3. (a) Selectivity change in p-CNB hydrogenation on serial Pt/CeO2 catalysts with different Pt loadings. (b) The energy barriers (Ea) of dehalogenation for p-CAN versus the cone angle of Pt on Pt-based catalyst models. (c) The 0.005 e-/Å3isosurfaces of C-Cl π* orbitals (unoccupied) and non-bonding orbitals of Cl in p-CAN molecule. (d-f) The orbital analysis between p-CAN and different coordinated Pt sites: (d) Pt1/CeO2; (e) Pt/(111); (f) Pt-edge. (g) High-resolution valence-band Pt 5d XPS in different sized-Pt/SiO2 relative to the VBM, as an analogue of the density of states. Positions of the d-band centers was indicated as the black lines. (h) The corresponding catalytic activities in hydrogenation of quinoline at room temperature and ambient (balloon) hydrogen pressure against diameter of the PtNPs. Panels (a)-(f) reproduced with permission from Ref. [30]. Copyright 2020, Elsevier. Panels (g) and (h) reproduced with permission Ref. [62]. Copyright 2016, Wiley.

Fig. 4. (a) Sketch maps of metal nanoparticles in different shape: tetrahedron (a1), octahedron (a2), cube (a3) and cuboctahedron (a4). The tetrahedron and octahedron only exhibit the (111) facets. Reproduced with permission from Ref. [65]. Copyright 2010, American Chemical Society. (b,c). Schematic of different surfaces in face-centered cubic (FCC) and body-centered cubic (BCC) lattice. (b1) (111), (b2) (100) and (b3) (110) of FCC. (c1) (111), (c2) (100) and (c3) (110) of BCC.

Fig. 5. TEM images of Pd1/Cu (111) (a) and Pd1/Cu (100) (b); (c) Hydrogenation activity of Cu(100) and Cu(111) surface supported single-atom Pd with varied Pd loading; (d) Evolution of the onset temperature for 2-propanol oxidation over Pt NPs/γ-Al2O3 versus the average number of missing bonds (related to the population of low-coordinated atoms) on the NP surface; (e) The percentage of atoms at corners/edges and faces on the NP surface, respectively. Panels (a)-(c) reproduced with permission from Ref. [69]. Copyright 2019 Springer Nature. Panels (d,e) reproduced with permission from Ref. [75]. Copyright 2010, American Chemical Society.

Fig. 6. (a) A synthetic scheme of Pt NSs/CNTs and Pt NPs/CNT; (b-d) HRTEM images of the periphery of intermediate Pt(OH)x/Pt species during the reduction process; (e-g) Polarization curves (scan rate: 50 mV/s), calculated TOF and number of active sites at the voltage of -0.1 V, and mass activity at a given voltammetry over different shaped-Pt catalysts. Reproduced with permission from Ref. [71]. Copyright 2020, Elsevier.

Table 1 Catalytic performance of metal/N-doped carbon catalysts employed for various heterogeneous reactions.

Entry	Catalyst	Application	Performance ^a	Ref.
1	Pd/CN_0.132	Hydride oxygenation of vanillin	con. 100%, sel. 100%	[100]
2	Pd/AC		con. 98%, sel. 74%	[100]
3	Pd/HPC-NH₂		con.100%, sel. 99.3%	[101]
4	Pd/HPC		no-reactivity	[101]
5	Pd/NPC-ZIF-8		TOF 100 h^-1	[102]
6	Pd/AC		TOF 22 h^-1	[102]
7	PdZn/CN@ZnO	Semi hydrogenation of alkynols	TOF 434 h^-1	[103]
8	PdZn/ZnO	Semi hydrogenation of alkynols	TOF 74 h^-1	[103]
9	Pd/CN@MgO	aldol condensation- hydrogenation of furfural	con. > 99%, sel. 82%	[104]
10	Pd/MgO	aldol condensation- hydrogenation of furfural	con. 86%, sel. 42%	[104]

Fig. 7. (a) Adsorption configurations of metal particles and corresponding adsorption energies of NPs on different carbon supports. GP: undoped graphene; NG: Ng doped-graphene; PNG: Np doped-graphene. The scheme of the electron transfer between NPs and different carbon supports. Blue means occupied electrons. The values represent Fermi levels against the vacuum. White circle denotes the electron deficiency of the carbon atoms bound to Ng. (b) Catalytic performance of Pd-based catalysts over different supports in the additive-free dehydrogenation of FA; (c) XPS spectra of Pd 3d for Pd-based catalysts on varied supports; (d) Possible reaction pathway for the dehydrogenation of FA over Pd/NHPC-NH2. Panels (a-c) reproduced with permission from Ref. [105]. Copyright 2019, Elsevier. Panels (d-f) reproduced from Ref. [107]. Copyright 2019, Royal Society of Chemistry.

Fig. 8. Calculated energy profiles of C-O bond cleavage of C4H9OH (a) and C6H5OH (b) over NbOPO4(100) (black line) and Re2O7(010) (red line) surfaces, respectively. (c) The isosurfaces of charge density difference for O and OH adsorption on NbOPO4(100) and Re2O7(010) surfaces. (d) The d-orbital projected density of states for the surface Nb5c and Re5c atoms. Panels (a)-(d) were all adapted with permission from Ref. [125]. Copyright 2016, Springer Nature. High resolution STEM Z-contrast image of 2%Pt/α-MoC (e) and 0.2%Pt/α-MoC (f) with the single Pt atoms circled; (g) The catalytic activity of based Pt/MoC samples with a changed molar percentage of α-MoC and the corresponding fitted coordination numbers of Pt-Pt and Pt-Mo shells; (h) The long-term stability of the 0.2%Pt/α-MoC catalysts. Reaction was carried in the condition of n(CH3OH):n(H2O)= 1:1. TTN, total turnover number. Panels (e)-(h) were all adapted with permission from Ref. [128]. Copyright 2017, Springer Nature.

Fig. 9. (a) Schematic representation of main metal-support interactions between metal NPs and supports; XPS spectra of single Pt atom over Co3O4, CeO2, ZrO2 and graphene in the Pt 4f region (b) and the corresponding catalytic performance of Pt1 SACs in hydrolytic dehydrogenation of ammonia borane for room-temperature (c). Panels (b) and (c) reproduced with permission from Ref. [130] Copyright 2019, American Chemical Society. (d) Representative HRTEM images of an individual Pd nanocrystal supported on In2O3 under reducing atmospheres; (e) The catalytic performance of Pd/In2O3 catalysts treated at different reduction temperatures in the MBY semi-hydrogenation reaction. Panels (d) and (e) adapted with permission from Ref [109]. Copyright 2019, Royal Society of Chemistry. (f) Calculated fraction of sites with a specific geometry (surface and perimeter or corner atoms in contact with the support) and turnover frequency (TOF) based on the total metal atom for CO oxidation on CeO2 supported Ni, Pd, and Pt catalysts as a function of metal particle size. Adapted with permission from Ref. [131] Copyright 2013, Science AAAS.

Fig. 10. (a) Structure diagram of geometrical effects caused by alloying affect; (b) In situ infrared spectra over the Pt/Al2O3 and PtSn/Al2O3 during PDH reaction. The mainly pathways including dehydrogenation and cracking and the corresponding reaction energy of the steps catalyzed by Pt (111) and PtSn (102). Panels (b) adapted with permission from Ref. [172]. Copyright 2020, Wiley. (c) Energy Level illustration for Pt 5d Valence Bands in Pt/SiO2 and Pt1Zn1/SiO2 and the corresponding catalytic behavior in the ethane dehydrogenation reaction. Reproduced with permission from Ref. [177]. Copyright 2017, American Chemical Society.

Fig. 11. (a) The adsorption configuration model of HHDMA molecules on Pd(111). Reproduced with permission from Ref. [198]. Copyright 2014, Wiley. (b) Structured models of bare Pt NW and EDA-Pt NW and their corresponding Bader charge analysis; (c) Free energies for the adsorption of N-containing aromatics on the EDA-Pt NWs. Adapted with permission from Ref. [203]. Copyright 2016, Springer Nature.

Fig. 12. HAADF-STEM (a) and HRTEM (b) images of the as-prepared Pd/HPC-NH2. (c) The catalytic performance of Pd/HPC and Pd/HPC-NH2 in the hydrodeoxygenation of vanillin reaction using the FA as hydrogen source; (d) The conversion rate of benzaldehyde (BAL) under different HDO systems at 30 °C. The conversion rate was calculated based on the mass of Pd in Pd/HPC-NH2 catalyst at the conversion of ~10%. Panel (a)-(d) were reproduced with permission from Ref. [101]. Copyright 2021, Elsevier. HRTEM (e) and HAADF-STEM (f) images of Pd/NHPC-DETA-50; Catalytic selectivity (g) and activity (h) of the selective hydrogenation of MBY with different Pd catalysts. Adapted with permission from Ref. [206]. Copyright 2021, American Chemical Society.

Fig. 13. (a) In situ AC-STEM images of isolated Pt atom over TiO2 at different annealing conditions: 300 °C, 760 torr of O2 (a1); 250 °C, 760 torr of 5% H2 (a2); 450 °C, 760 torr of 5% H2 (a3). The same Pt single atom was identified by the yellow circles in the a1-a3. (a4) The normalized intensity profile of a line scan shown in (a1) and (a3). Panel (a) was adapted with permission from Ref [26]. Copyright 2019, Springer Nature. (b) In situ-ETEM images of Au/TiO2 and corresponding FFT patterns in different environments. (c) In situ-ETEM images showing the structural evolution of the Au-TiO2 under different reactive environment. Panels (b) and (c) reproduced with permission from Ref. [209]. Copyright 2021, Science AAAS.

Fig. 14. (a) Operando HERFD-XANES spectra of Pt-SS recorded at different temperatures under steady-state reaction conditions; (b) Catalytic activity during the HERFD-XANES experiments versus fraction of Pt4+, Pt2+, Ptδ+with adsorbed CO and the PtXδ+clusters, obtained by linear combination analysis using MCR-ALS as references; (c) Diagram for the reversible formation of the catalytically active PtXδ+cluster based on result of operando HERFD-XANES (grey, Pt; yellow, Ce; red, O; dark grey, C); (d) HERFD-XAS spectra of Pt-SS treated in different condition. MCR-ALS-derived references (e) and calculated HERFD-XANES (f) using relaxed Pt-SS structures on the 110 facet (indexed (i)-(iii)) and on the 111 facet (indexed (iv)) determined by DFT. Reproduced with permission from Ref. [221]. Copyright 2020, Springer Nature.

Fig. 15. The quasi in situ Pd 3d spectra for Pd NPs on AC (a) and CN (b) supports, and N 1s (c) before and after exposure in air. Panels (a)-(c) reproduced with permission from Ref. [105]. Copyright 2019, Elsevier. (d) In situ Pd 3d5/2 spectra of Pd foil under acetylene, propyne, and 1-pentyne selective hydrogenation; (e) Schematic representation of Pd catalysts operating in the selective and unselective alkyne hydrogenation regimes; (f) Relationship between Rh/Pd atomic fractions of as-synthesized Rh0.5Pd0.5 NPs and photoelectron KE and mean free path measured at 25 °C in UHV; (g) Evolution of Rh and Pd atomic fractions, the fraction of the oxidized Rh (left y axis) and Pd atoms (right y axis) in the Rh0.5Pd0.5 NPs at 300 °C under different conditions denoted in the x axis. Panels (d,e) and (f,g) were reproduced with permission from Ref [227] and Ref [232]. Copyright 2008, Science AAAS, respectively.

Fig. 16. (a) Catalytic performance of 3% Pt/CeO2 with different ratios of Pt/p-CNB. Infrared spectroscopy of CO adsorption on different catalysts: (b) fresh 3% Pt/CeO2 samples and used 3% Pt/CeO2 samples with Pt/p-CNB ratio of 2.3 wt‰ (c) and 31.7 wt‰ (d) in the reaction. Reproduced with permission from ref. [30]. Copyright 2020, Elsevier.

Fig. 17. In situ DRIFT spectra of CO adsorption and following O2 purging treatment over Pt/SiO2 and Pt/Al2O3 (a) and Pt/TiO2 and Pt/ZrO2 (b). (c,d) HAADF images of the as-synthesized 1 wt% Pt/SiO2. Arrows indicate the single atoms. Inset was the magnified image. (e) IR spectra of CO adsorbed over Pt/SiO2 before and after O2 treatment. The difference spectrum indicated the CO had been removed by O2; Kubelka-Munk unit is used for quantification. (f) CO2 signal in MS during the TPO process of the preadsorbed CO on Pt/SiO2. Reproduced with permission from Ref. [241]. Copyright 2015, Science AAAS.

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Coordination environment of active sites and their effect on catalytic performance of heterogeneous catalysts

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