Tuning the Adsorption Energy of Methanol Molecules Along Ni‐N‐Doped Carbon Phase Boundaries by the Mott–Schottky Effect for Gas‐Phase Methanol Dehydrogenation |
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| Authors: | Zhong‐Hua Xue Jing‐Tan Han Wei‐Jie Feng Qiu‐Ying Yu Prof Xin‐Hao Li Prof Markus Antonietti Prof Jie‐Sheng Chen |
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| Institution: | 1. School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, P. R. China;2. Department of Colloid Chemistry, Max Planck Institute of Colloids and Interfaces, Potsdam, Germany |
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| Abstract: | Engineering the adsorption of molecules on active sites is an integral and challenging part for the design of highly efficient transition‐metal‐based catalysts for methanol dehydrogenation. A Mott–Schottky catalyst composed of Ni nanoparticles and tailorable nitrogen‐doped carbon‐foam (Ni/NCF) and thus tunable adsorption energy is presented for highly efficient and selective dehydrogenation of gas‐phase methanol to hydrogen and CO even under relatively high weight hourly space velocities (WHSV). Both theoretical and experimental results reveal the key role of the rectifying contact at the Ni/NCF boundaries in tailoring the electron density of Ni species and enhancing the absorption energies of methanol molecules, which leads to a remarkably high turnover frequency (TOF) value (356 mol methanol mol?1 Ni h?1 at 350 °C), outpacing previously reported bench‐marked transition‐metal catalysts 10‐fold. |
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| Keywords: | adsorption energy gas– solid reactions heterogeneous catalysis Mott– Schottky effect nanostructures |
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