Reduction of Nitric Oxide with Hydrogen on Catalysts of Singly Dispersed Bimetallic Sites Pt1Com and Pd1Con

ACS CATALYSIS(2016)

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摘要
The bimetallic catalyst has been one of the main categories of heterogeneous catalysts for chemical production and energy transformation. Isolation of the continuously packed bimetallic sites of a bimetallic catalyst forms singly dispersed bimetallic sites which have distinctly different chemical environment and electronic state and thus exhibit a different catalytic performance. Two types of catalysts consisting of singly dispersed bimetallic sites Pt1Com or Pd1Con (m and n are the average coordination numbers of Co to a Pt or Pd atom) were prepared through a deposition or impregnation with a following controlled calcination and reduction to form Pt1Com or Pd1Con sites. These bimetallic sites are separately anchored on a nonmetallic support. Each site only consists of a few metal atoms. Single dispersions of these isolated bimetallic sites were identified with scanning transmission electron microscopy. Extended X-ray absorption fine structure spectroscopy (EXAFS) revealed the chemical bonding of single atom Pt-1 (or Pd-1) to Co atoms and thus confirmed the formation of bimetallic sites, Pt1Com and Pd1Con. Reduction of NO with H-2 was used as a probing reaction to test the catalytic performance on this type of catalyst. Selectivity in reducing nitric oxide to N-2 on Pt1Com at 150 degrees C is 98%. Pd1Con is active for reduction of NO with a selectivity of 98% at 250 degrees C. In situ studies of surface chemistry with ambient-pressure X-ray photoelectron spectroscopy and coordination environment of Pt and Pd atoms with EXAFS showed that chemical state and coordination environment of Pt1Com and Pd1Con remain during catalysis up to 250 and 300 degrees C, respectively. The correlation of surface chemistries and structures of these catalysts with their corresponding catalytic activities and selectivities suggests a method to develop new bimetallic catalysts and a new type of single site catalysts.
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bimetallic,exafs
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