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Designing Sites in Heterogeneous Catalysis: Are We Reaching Selectivities Competitive With Those of Homogeneous Catalysts?

期刊

CHEMICAL REVIEWS
卷 122, 期 9, 页码 8594-8757

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.chemrev.1c00905

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资金

  1. U.S. National Science Foundation [1953843, 1854439]
  2. U.S. Department of Energy [DESC0001839]
  3. Direct For Mathematical & Physical Scien
  4. Division Of Chemistry [1854439, 1953843] Funding Source: National Science Foundation

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This article provides a critical review of various prominent nanotechnologies used in catalysis, focusing on how they contribute to improving selectivity in heterogeneous catalysis. The ways to modify catalytic sites include reversible or irreversible adsorption of molecular modifiers, immobilization or tethering of homogeneous catalysts, and the development of well-defined catalytic sites on solid surfaces. These methodologies have advantages and limitations, but they offer new possibilities for catalyst design in specific applications.
A critical review of different prominent nanotechnologies adapted to catalysis is provided, with focus on how they contribute to the improvement of selectivity in heterogeneous catalysis. Ways to modify catalytic sites range from the use of the reversible or irreversible adsorption of molecular modifiers to the immobilization or tethering of homogeneous catalysts and the development of well-defined catalytic sites on solid surfaces. The latter covers methods for the dispersion of single-atom sites within solid supports as well as the use of complex nanostructures, and it includes the post-modification of materials via processes such as silylation and atomic layer deposition. All these methodologies exhibit both advantages and limitations, but all offer new avenues for the design of catalysts for specific applications. Because of the high cost of most nanotechnologies and the fact that the resulting materials may exhibit limited thermal or chemical stability, they may be best aimed at improving the selective synthesis of high value-added chemicals, to be incorporated in organic synthesis schemes, but other applications are being explored as well to address problems in energy production, for instance, and to design greener chemical processes. The details of each of these approaches are discussed, and representative examples are provided. We conclude with some general remarks on the future of this field.

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