Efficient subnanometric gold-catalyzed hydrogen generation via formic acid decomposition under ambient conditions

Journal of the American Chemical Society
Qing-Yuan BiKang-Nian Fan

Abstract

Formic acid (FA) has tremendous potential as a safe and convenient source of hydrogen for sustainable chemical synthesis and renewable energy storage, but controlled and efficient dehydrogenation of FA by a robust solid catalyst under ambient conditions constitutes a major challenge. Here, we report that a previously unappreciated combination of subnanometric gold and an acid-tolerant oxide support facilitates the liberation of CO-free H(2) from FA. Applying an ultradispersed gold catalyst comprising TEM-invisible gold subnanoclusters deposited on zirconia to a FA-amine mixture affords turnover frequencies (TOFs) up to 1590 per hour and a turnover number of more than 118,400 at 50 °C. The reaction was accelerated at higher temperatures, but even at room temperature, a significant H(2) evolution (TOFs up to 252 h(-1) after 20 min) can still be obtained. Preliminary mechanistic studies suggest that the reaction is unimolecular in nature and proceeds via a unique amine-assisted formate decomposition mechanism on Au-ZrO(2) interface.

References

Nov 20, 2001·Nature·L Schlapbach, A Züttel
Apr 15, 2004·Angewandte Chemie·Masakazu DatéMasatake Haruta
Nov 4, 2004·Angewandte Chemie·Massimiliano ComottiMichele Rossi
Sep 14, 2006·Chemical Reviews·George W HuberAvelino Corma
Oct 10, 2006·Chemical Communications : Chem Comm·Daljit S MatharuMartin Wills
Aug 19, 2007·Angewandte Chemie·Tamao Ishida, Masatake Haruta
Aug 25, 2007·Chemical Reviews·R M NavarroJ L G Fierro
Jul 26, 2008·Chemical Communications : Chem Comm·Xiaochun ZhouTianhong Lu
Aug 8, 2008·ChemSusChem·Albert BoddienMatthias Beller
Sep 11, 2008·ChemSusChem·Stephan Enthaler
Nov 6, 2008·ChemSusChem·Kai Man Kerry YuShik Chi Edman Tsang
Jan 16, 2009·Angewandte Chemie·Karaked TedsreeShik Chi Tsang
Feb 21, 2009·Chemistry : a European Journal·Céline FellayGábor Laurenczy
May 30, 2009·Angewandte Chemie·Manuel Ojeda, Enrique Iglesia
Dec 22, 2009·Chemical Society Reviews·Tarn C JohnsonMartin Wills
Mar 20, 2010·ChemSusChem·Artur MajewskiMartin Wills
Jun 17, 2010·Journal of the American Chemical Society·Albert BoddienMatthias Beller
Aug 3, 2010·Chemical Reviews·Anne StaubitzIan Manners
Nov 10, 2010·Journal of the American Chemical Society·Peter HauwertCornelis J Elsevier
May 24, 2011·Angewandte Chemie·Albert BoddienMatthias Beller
Jul 12, 2011·Journal of the American Chemical Society·Gerrit WienhöferMatthias Beller
Sep 24, 2011·Science·Albert BoddienMatthias Beller
Nov 8, 2011·Angewandte Chemie·Debora PretiGiuseppe Fachinetti

❮ Previous
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Citations

Dec 18, 2013·Accounts of Chemical Research·Xiang LiuYong Cao
Apr 15, 2016·Nature Communications·Jeff Joseph A CelajeTravis J Williams
Mar 31, 2017·Chemical Communications : Chem Comm·Yulu ZhanXiaochun Zhou
Feb 16, 2017·Chemical Communications : Chem Comm·Liang WangFeng-Shou Xiao
Mar 24, 2016·Physical Chemistry Chemical Physics : PCCP·Nan He, Zhen Hua Li
Nov 23, 2016·Chemical Communications : Chem Comm·Dong WangMianheng Jiang
Oct 27, 2016·Physical Chemistry Chemical Physics : PCCP·Ming-Xing LiangHai-Shun Wu
Jun 12, 2018·Chemical Communications : Chem Comm·Zhiyao LuTravis J Williams
Aug 1, 2015·Chemistry : a European Journal·Ying JiaEugene Pinkhassik
Aug 3, 2017·Chemistry : a European Journal·Elena PedrajasRosa Llusar
Sep 14, 2017·Angewandte Chemie·Roopender KumarCristina Nevado
Apr 3, 2019·Chemistry : a European Journal·Wei ZhouMatthias Beller
Sep 21, 2013·Chemical Communications : Chem Comm·Yu-ling QinXin-bo Zhang
Aug 28, 2019·Nanoscale·Michelle MuzzioShouheng Sun
Sep 24, 2019·Faraday Discussions·Nitish Govindarajan, Evert Jan Meijer
Feb 23, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Karan ChaudharyNigam P Rath
Feb 8, 2020·Chemistry, an Asian Journal·Chao GuanKuo-Wei Huang

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