Spatially isolated dual-active sites enabling selective hydrogenation
Source abstract
Abstract
Rational design of heterogeneous catalysts with dual-active sites provides a strategy to achieve efficient and selective hydrogenation under mild conditions by breaking the restriction of Brønsted-Evans-Polanyi scaling relations. Steric hindrance effects by encapsulating active components inside porous shells have been widely adopted to design catalysts with dual-active sites for selective hydrogenation. However, this methodology is always at the cost of the limited catalytic activity due to the restricted mass transfer through porous shell and inevitable sacrifice of part of the active sites inside shells. This perspective illustrates dual-active sites on the surface of supported metal catalysts, enabling simultaneously improved activity and selectivity for various hydrogenations. The key discussions include experimental evidence, construction guidelines, successful cases, and potential influencing factors of selective hydrogenation for constructing dual-active sites on the metal-supported catalysts. This perspective offers valuable insights into future prospects to stimulate and guide the design of advanced catalysts for selective hydrogenation.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Nanomaterials for catalytic reactions · Asymmetric Hydrogenation and Catalysis · Catalysis and Hydrodesulfurization Studies
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (100+)
Show source-provided references
1. Surface and interface coordination chemistry learned from model heterogeneous metal nanocatalysts: From atomically dispersed catalysts to atomically precise clusters10.1021/acs.chemrev.2c00569 ↗
2. Chemical synthesis of single atomic site catalysts10.1021/acs.chemrev.9b00818 ↗
3. Single-atom catalysts across the periodic table10.1021/acs.chemrev.0c00576 ↗
4. Chemical and thermal sintering of supported metals with emphasis on cobalt catalysts during Fischer-Tropsch synthesis10.1021/acs.chemrev.9b00417 ↗
5. Surface and interface control in nanoparticle catalysis10.1021/acs.chemrev.9b00220 ↗
6. Catalyst: Single-atom catalysis: Directing the way toward the nature of catalysis10.1016/j.chempr.2019.10.004 ↗
7. Selective hydrogenation over supported metal catalysts: From nanoparticles to single atoms10.1021/acs.chemrev.9b00230 ↗
8. Guidelines to achieving high selectivity for the hydrogenation of alpha,beta-unsaturated aldehydes with bimetallic and dilute alloy catalysts: A review10.1021/acs.chemrev.0c00582 ↗
9. Recent progress in heterogeneous asymmetric hydrogenation of C=O and C=C bonds on supported noble metal catalysts10.1021/acs.chemrev.7b00272 ↗
10. Heterogeneous catalysis: A central science for a sustainable future10.1021/acs.accounts.6b00510 ↗
11. Reactivity theory of transition-metal surfaces: A Brønsted−Evans−Polanyi linear activation energy−free-energy analysis10.1021/cr9001808 ↗
12. Modeling ethanol decomposition on transition metals: A combined application of scaling and Bronsted-Evans-Polanyi relations10.1021/ja8099322 ↗
13. The Brønsted–Evans–Polanyi relation and the volcano curve in heterogeneous catalysis10.1016/j.jcat.2004.02.034 ↗
14. Advances in the design of nanostructured catalysts for selective hydrogenation10.1002/cctc.201501269 ↗
15. Surface molecular imprinting over supported metal catalysts for size-dependent selective hydrogenation reactions10.1038/s41929-021-00649-3 ↗
16. Insights into the interfacial effects in heterogeneous metal nanocatalysts toward selective hydrogenation10.1021/jacs.0c13185 ↗
17. Recent progress in Pd-based nanocatalysts for selective hydrogenation10.1021/acsomega.1c06244 ↗
18. Metal single-atom catalysts for selective hydrogenation of unsaturated bonds10.1039/D1TA00022E ↗
19. Mechanistic understanding and the rational design of sinter-resistant heterogeneous catalysts10.1021/acscatal.7b01975 ↗
20. Single-atom catalyst: a rising star for green synthesis of fine chemicals10.1093/nsr/nwy077 ↗
21. Well-defined materials for heterogeneous catalysis: From nanoparticles to isolated single-atom sites10.1021/acs.chemrev.9b00311 ↗
22. Single-atom alloy catalysis10.1021/acs.chemrev.0c00078 ↗
23. Single-atom catalysts based on the metal-oxide interaction10.1021/acs.chemrev.0c00797 ↗
24. Mechanochemical kilogram-scale synthesis of noble metal single-atom catalysts10.1016/j.xcrp.2019.100004 ↗
25. Single atom is not alone: Metal–support interactions in single-atom catalysis10.1016/j.mattod.2020.07.002 ↗
26. Surface coordination chemistry of atomically dispersed metal catalysts10.1021/acs.chemrev.0c00094 ↗
27. Highly selective hydrogenation of phenol and derivatives over a Pd@carbon nitride catalyst in aqueous media10.1021/ja109856y ↗
28. Hydrogen spillover through Matryoshka-type (ZIFs@)n-1ZIFs nanocubes10.1038/s41467-018-06269-z ↗
29. Metal-organic frameworks as selectivity regulators for hydrogenation reactions10.1038/nature19763 ↗
30. Product selectivity controlled by nanoporous environments in zeolite crystals enveloping rhodium nanoparticle catalysts for CO2 hydrogenation10.1021/jacs.9b01555 ↗
31. Activation and spillover of hydrogen on sub-1 nm palladium nanoclusters confined within sodalite zeolite for the semi-hydrogenation of alkynes10.1002/anie.201903827 ↗
32. A Pd@Zeolite catalyst for nitroarene hydrogenation with high product selectivity by sterically controlled adsorption in the zeolite micropores10.1002/anie.201703938 ↗
33. Elucidating the roles of amorphous alumina overcoat in palladium-catalyzed selective hydrogenation10.1021/acsami.2c02132 ↗
34. Magic of hydrogen spillover: Understanding and application10.1016/j.gee.2022.01.013 ↗
35. Hydrogen spillover. Facts and fiction10.1021/cr200346z ↗
36. The hydrogen spillover effect. A misunderstanding story10.1080/01614940.2020.1787771 ↗
37. New sorbents for hydrogen storage by hydrogen spillover – a review10.1039/b807957a ↗
38. Spillover in heterogeneous catalysis: New insights and opportunities10.1021/acscatal.0c05567 ↗
39. Hydrogen spillover in the Fischer-Tropsch synthesis on carbon-supported cobalt catalysts10.1002/cctc.201901934 ↗
40. Controlling a spillover pathway with the molecular cork effect10.1038/nmat3620 ↗
41. Water-mediated proton hopping on an iron oxide surface10.1126/science.1219468 ↗
42. Catalyst support effects on hydrogen spillover10.1038/nature20782 ↗
43. The long and winding road to catalysis10.1038/541037a ↗
44. Dual-active-sites design of Co@C catalysts for ultrahigh selective hydrogenation of N-heteroarenes10.1016/j.chempr.2020.07.023 ↗
45. Single-atom engineering to ignite 2D transition metal dichalcogenide based catalysis: Fundamentals, progress, and beyond10.1021/acs.chemrev.1c00505 ↗
46. Theoretical understanding of the stability of single-atom catalysts10.1093/nsr/nwy094 ↗
47. Isolated metal atom geometries as a strategy for selective heterogeneous hydrogenations10.1126/science.1215864 ↗
48. Boosting activity and stability of metal single-atom catalysts via regulation of coordination number and local composition10.1021/jacs.1c09498 ↗
49. Hydrogen spillover and its relation to hydrogenation: observations on structurally defined single-atom sites
50. In-situ reconstruction of single-atom Pt on Co3O4 for hydrogenation10.1007/s12274-022-5279-1 ↗
51. Spatial intimacy of binary active-sites for selective sequential hydrogenation-condensation of nitriles into secondary imines10.1038/s41467-021-23705-9 ↗
52. Optimum particle size for gold-catalyzed CO oxidation10.1021/acs.jpcc.7b12711 ↗
53. Exploring the materials space in the smallest particle size range: from heterogeneous catalysis to electrocatalysis and photocatalysis10.1039/D1CP05677H ↗
54. Size-dependent adsorption of styrene on Pd clusters: A density functional theory study10.1021/acs.jpcc.8b09477 ↗
55. Site-specific reactivity of molecules with surface defects-the case of H2 dissociation on Pt10.1126/science.aau6716 ↗
56. Three-site model for hydrogen adsorption on supported platinum particles: Influence of support ionicity and particle size on the hydrogen coverage10.1021/ja045286c ↗
57. Adsorption and diffusion of hydrogen on the surface of the Pt24 subnanoparticle. A DFT study10.1021/acs.jpcc.6b04555 ↗
58. High catalytic activity and chemoselectivity of sub-nanometric Pd clusters on porous nanorods of CeO2 for hydrogenation of nitroarenes10.1021/jacs.5b11413 ↗
59. Low pressure induced porous nanorods of ceria with high reducibility and large oxygen storage capacity: synthesis and catalytic applications10.1039/C4TA03718A ↗
60. Visible-light-activated Suzuki–Miyaura coupling reactions of aryl chlorides over the multifunctional Pd/Au/porous nanorods of CeO2 catalysts10.1021/acscatal.5b01173 ↗
61. Sustainable production of hydrogen with high purity from methanol and water at low temperatures10.1038/s41467-022-33186-z ↗
62. Platinum and frustrated Lewis pairs on ceria as dual-active sites for efficient reverse water-gas shift reaction at low temperatures
63. Solid frustrated-Lewis-pair catalysts constructed by regulations on surface defects of porous nanorods of CeO2
64. Interfacial frustrated Lewis pairs of CeO2 activate CO2 for selective tandem transformation of olefins and CO2 into cyclic carbonates10.1021/jacs.9b03217 ↗
65. Highly selective transfer hydrogenation of furfural into furfuryl alcohol by interfacial frustrated Lewis pairs on CeO210.1016/j.jcat.2022.04.010 ↗
66. Metal catalysts for heterogeneous catalysis: From single atoms to nanoclusters and nanoparticles10.1021/acs.chemrev.7b00776 ↗
67. Insight into single-atom-induced unconventional size dependence over CeO2-supported Pt catalysts10.1016/j.chempr.2019.12.029 ↗
68. Competition of C-C bond formation and C-H bond formation For acetylene hydrogenation on transition metals: A density functional theory study10.1002/aic.16492 ↗
69. Electronic state regulation of supported Pt catalysts dictates selectivity of imines/secondary amines from the cascade transformation of nitroarenes and aldehydes10.1016/j.apcatb.2019.118451 ↗
70. Mechanistic insights on the hydrogenation of α,β-unsaturated ketones and aldehydes to unsaturated alcohols over metal catalysts10.1021/cs200567z ↗
71. Selective hydrogenation of cinnamaldehyde over Co-based intermetallic compounds derived from layered double hydroxides10.1021/acscatal.8b02755 ↗
72. Cooperation of Pt and TiOx in the hydrogenation of nitrobenzothiazole10.1021/acscatal.2c02988 ↗
73. The surface chemistry of metal-based hydrogenation catalysis10.1021/acscatal.7b01368 ↗
74. Boosting selective hydrogenation through hydrogen spillover on supported-metal catalysts at room temperature10.1016/j.apcatb.2021.120418 ↗
75. Highly selective catalysts for the hydrogenation of unsaturated aldehydes: A review10.1021/acscatal.9b04331 ↗
76. Recent advances in selective hydrogenation of cinnamaldehyde over supported metal-based catalysts10.1021/acscatal.9b05031 ↗
77. Heterogeneous hydrogenation with hydrogen spillover enabled by nitrogen vacancies on boron nitride-supported Pd nanoparticles
78. Hydrogen spillover to oxygen vacancy of TiO2-xHy/Fe: Breaking the scaling relationship of ammonia synthesis10.1021/jacs.0c06118 ↗
79. Effects of Co and Ru intimacy in Fischer–Tropsch catalysts using hollow carbon sphere supports: Assessment of the hydrogen spillover processes10.1021/acscatal.6b03102 ↗
80. Disentangling local interfacial confinement and remote spillover effects in oxide-oxide interactions10.1021/jacs.3c02483 ↗
81. Ultrahigh selective hydrogenation of furfural enabled by modularizing hydrogen dissociation and substrate activation10.1021/acscatal.3c01506 ↗
82. Dual metal nanoparticles within multicompartmentalized mesoporous organosilicas for efficient sequential hydrogenation10.1038/s41467-021-25226-x ↗
83. On the mechanism of H2 activation over single-atom catalyst: An understanding of Pt1/WOx in the hydrogenolysis reaction10.1016/S1872-2067(19)63517-5 ↗
84. Pt, Ir, Ru, and Rh nanoparticles supported on ZIF-67 nanocubes for evaluation of hydrogen spillover ability of noble metals10.1021/acsanm.1c00871 ↗
85. Separating catalytic activity at edges and terraces on platinum: Hydrogen dissociation10.1021/jp401355c ↗
86. Hydrogen adsorption, dissociation, and spillover on Ru10 clusters supported on anatase TiO2 and Tetragonal ZrO2 (101) surfaces10.1021/acscatal.5b01093 ↗
87. Tuning the Pt/CeO2 interface by in situ variation of the Pt particle size10.1021/acscatal.8b00330 ↗
88. Investigation of the support effect in atomically dispersed Pt on WO3-x for utilization of Pt in the hydrogen evolution reaction10.1002/anie.201908122 ↗
89. Low-temperature CO2 methanation over CeO2-supported Ru single atoms, nanoclusters, and nanoparticles competitively tuned by strong metal–support interactions and H-spillover effect10.1021/acscatal.7b04469 ↗
90. Modifying interface of carbon support-stimulated hydrogen spillover for selective hydrogenation10.1021/acs.jpcc.2c05438 ↗
91. Facet engineering accelerates spillover hydrogenation on highly diluted metal nanocatalysts10.1038/s41565-020-0746-x ↗
92. On the mechanisms of hydrogen spillover in MoO310.1021/jp7119137 ↗
93. Hydrogen spillover-accelerated selective hydrogenation on WO3 with ppm-level Pd10.1021/acsami.3c00456 ↗
94. Improving the efficiency of hydrogen spillover by an organic molecular decoration strategy for enhanced catalytic hydrogenation performance10.1021/acscatal.2c06074 ↗
95. The mechanism of spillover of hydrogen on sp2-carbon surface10.1080/1536383X.2019.1708732 ↗
96. The theoretical study of the bimetallic Ni/Pd, Ni/Pt and Pt/Pd catalysts for hydrogen spillover on penta-graphene10.1016/j.ijhydene.2018.08.143 ↗
97. Hydrogen spillover in Pt-single-walled carbon nanotube composites: formation of stable C-H bonds10.1021/ja200403m ↗
98. Tuning the interfaces in the ruthenium-nickel/carbon nanocatalysts for enhancing catalytic hydrogenation performance10.1016/j.jcat.2019.07.041 ↗
99. Mechanism of hydrogen spillover on WO3(001) and formation of HxWO3 (x = 0.125, 0.25, 0.375, and 0.5)10.1021/jp410244c ↗
100. Highly efficient hydrogenation of nitrobenzene to aniline over Pt/CeO2 catalysts: The shape effect of the support and key role of additional Ce3+ sites10.1021/acscatal.0c02730 ↗