Polymer electrolyte membrane fuel cells (PEMFCs) running on hydrogen are attractive alternative power supplies for a range of applications1,2,3, with in situ release of the required hydrogen from a stable liquid offering one way of ensuring its safe storage and transportation4,5 before use. The use of methanol is particularly interesting in this regard, because it is inexpensive and can reform itself with water to release hydrogen with a high gravimetric density of 18.8 per cent by weight. But traditional reforming of methanol steam operates at relatively high temperatures (200–350 degrees Celsius)6,7,8, so the focus for vehicle and portable PEMFC applications9 has been on aqueous-phase reforming of methanol (APRM). This method requires less energy, and the simpler and more compact device design allows direct integration into PEMFC stacks10,11. There remains, however, the need for an efficient APRM catalyst. Here we report that platinum (Pt) atomically dispersed on α-molybdenum carbide (α-MoC) enables low-temperature (150–190 degrees Celsius), base-free hydrogen production through APRM, with an average turnover frequency reaching 18,046 moles of hydrogen per mole of platinum per hour. We attribute this exceptional hydrogen production—which far exceeds that of previously reported low-temperature APRM catalysts—to the outstanding ability of α-MoC to induce water dissociation, and to the fact that platinum and α-MoC act in synergy to activate methanol and then to reform it.
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We received financial support from the 973 Project (grants 2011CB201402 and 2013CB933100) and the Natural Science Foundation of China (grants 91645115, 21473003, 91645115, 21222306, 21373037, 21577013 and 91545121). The electron-microscopy work was supported in part by the Chinese Academy of Sciences (CAS) Pioneer Hundred Talents Program; by the US Department of Energy (DOE), Office of Science, Basic Energy Science, Materials Sciences and Engineering Division (to W.Z.); and through a user project at Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences (CNMS), which is a DOE Office of Science User Facility. The XAS experiments were conducted in the Shanghai Synchrotron Radiation Facility (SSRF) and Beijing Synchrotron Radiation Facility (BSRF). This research used Beamline 17-BM of the Advanced Photon Source (APS), a US DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357 (to W.X.). We also acknowledge National Thousand Young Talents Program of China the CAS Hundred Talents Program and the Shanxi Hundred Talent Program.
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In Situ Catalytic Etching Strategy Promoted Synthesis of Carbon Nanotube Inlaid with Ultrasmall FeP Nanoparticles as Efficient Electrocatalyst for Hydrogen Evolution
ACS Sustainable Chemistry & Engineering (2019)