Deoxydehydration with Molecular Hydrogen over Ceria-Supported Rhenium Catalyst with Gold Promoter

Deoxydehydration with Molecular Hydrogen over Ceria-Supported Rhenium Catalyst with Gold Promoter
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DOI:
10.1021/acscatal.6b01864
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发表时间:
2016-08
期刊:
影响因子:
12.9
通讯作者:
Shuhei Tazawa;Nobuhiko Ota;M. Tamura;Y. Nakagawa;K. Okumura;K. Tomishige
Shuhei Tazawa;Nobuhiko Ota;M. Tamura;Y. Nakagawa;K. Okumura;K. Tomishige
中科院分区:
化学1区
文献类型:
--
作者:
Shuhei Tazawa;Nobuhiko Ota;M. Tamura;Y. Nakagawa;K. Okumura;K. Tomishige

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金纳米颗粒助催化剂和二氧化铈载体催化剂使得能够使用H2作为Re催化脱氧脱水(DODH)的还原剂,将邻位二醇转化为烯烃,其活性高于使用非H2还原剂的均相Re催化剂,并且具有相当的选择性。ReOx-Au/CeO 2催化剂中合适的Au颗粒尺寸(约10 nm)对于活化H2同时保留DODH产物中的C → C键特别有效。甘油转化为烯丙醇的产率为91%,且每Re原子的TON达到300。该系统适用于其它底物,如丁二烯(1,3-丁二烯的产率为81%)。
Gold nanoparticle cocatalyst and ceria support catalyst enabled the use of H2 as a reductant for Re-catalyzed deoxydehydration (DODH), converting vicinal diols to olefins with higher activity than homogeneous Re catalysts using non-H2 reductants and with comparable selectivity. The suitable particle size (∼10 nm) of Au in ReOx-Au/CeO2 catalyst was especially effective for activating H2 while retaining the C═C bond in DODH products. Glycerol was converted to allyl alcohol in 91% yield, and the TON per Re atom reached 300. This system is applicable to other substrates such as erythritol (81% yield of 1,3-butadiene).