期刊
ACS CATALYSIS
卷 10, 期 12, 页码 6763-6770出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b04070
关键词
core-shell nanoparticles; carbides; nitrides; electronic structure; acetylene semihydrogenation
资金
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0016214]
- Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division, Catalysis Sciences Program [DE-SC0016192]
- US National Science Foundation (NSF) [CBET-1748365]
- Computational Materials Education and Training (CoMET) NSF Research Traineeship [DGE-1449785]
- National Science Foundation [ACI-1548562]
- DOE office of Sceince [De-AC0206CH11357, GUP 55290]
- Chyn Duog Shiah Memorial Fellowship
- U.S. Department of Energy (DOE) [DE-SC0016192] Funding Source: U.S. Department of Energy (DOE)
We demonstrate that atomically thin Pt shells deposited on transition metal carbide or nitride cores induce up to a 4-fold enhancement in C2H4 selectivity during the partial hydrogenation of acetylene compared with commercial carbon-supported Pt (Pt-comm) nanoparticles. While Pt typically catalyzes the complete hydrogenation of alkynes to alkanes, a catalyst comprising a nominal one monolayer (ML) Pt shell on titanium tungsten nitride cores (Pt/TiWN) is capable of net C2H4 generation under industrial front-end reaction conditions featuring a large excess of C2H4 and H-2. Microcalorimetry measurements are consistent with a change in the Pt electronic structure that decreases C2H4 binding strength, thus increasing partial hydrogenation selectivity. Density functional theory (DFT) calculations and X-ray absorption near edge structure (XANES) both indicate broadening of the Pt d-band and concomitant down-shifting of the d-band center. The ability to control shell coverage and core composition opens up extensive opportunities to modulate the electronic and catalytic properties of noble metal-based catalysts.
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