journal article·2017-05-23

Low-temperature Synthesis of Heterostructures of Transition Metal Dichalcogenide Alloys (WxMo1–xS2) and Graphene with Superior Catalytic Performance for Hydrogen Evolution

Yu Lei, Srimanta Pakhira, Kazunori Fujisawa, Xuyang Wang, Oluwagbenga Oare Iyiola, Néstor Perea López, Ana Laura Elías, Lakshmy Pulickal Rajukumar, Chanjing Zhou, Bernd Kabius, Nasim Alem, Morinobu Endo, Ruitao Lv, Jose L. Mendoza-Cortes, Mauricio Terrones

ACS Nano· Volume 11· Issue 5
Publisher page

Abstract

Large-area (∼cm 2 ) films of vertical heterostructures formed by alternating graphene and transition-metal dichalcogenide (TMD) alloys are obtained by wet chemical routes followed by a thermal treatment at low temperature. In particular, we synthesized stacked graphene and W x Mo 1– x S 2 alloy phases that were used as hydrogen evolution catalysts. We observed a Tafel slope of 38.7 mV dec –1 and 96 mV onset potential (at current density of 10 mA cm –2 ) when the heterostructure alloy was annealed at 300 °C. These results indicate that heterostructures formed by graphene and W 0.4 Mo 0.6 S 2 alloys are far more efficient than WS 2 and MoS 2 by at least a factor of 2, and they are superior compared to other reported TMD systems. This strategy offers a cheap and low temperature synthesis alternative able to replace Pt in the hydrogen evolution reaction (HER). Furthermore, the catalytic activity of the alloy is stable over time, i.e., the catalytic activity does not experience a significant change even after 1000 cycles. Using density functional theory calculations, we found that this enhanced hydrogen evolution in the W x Mo 1– x S 2 alloys is mainly due to the lower energy barrier created by a favorable overlap of the d-orbitals from the transition metals and the s-orbitals of H 2; with the lowest energy barrier occurring for the W 0.4 Mo 0.6 S 2 alloy. Thus, it is now possible to further improve the performance of the “inert” TMD basal plane via metal alloying, in addition to the previously reported strategies such as creation of point defects, vacancies and edges. The synthesis of graphene/W 0.4 Mo 0.6 S 2 produced at relatively low temperatures is scalable and could be used as an effective low cost Pt-free catalyst.
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Research context

OpenAlex topics: 2D Materials and Applications · Chalcogenide Semiconductor Thin Films · MXene and MAX Phase Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Materials Science and Engineering & Materials Research Institute, The Pennsylvania State University, University Park, Pennsylvania 16802, United States

Department of Chemical & Biomedical Engineering, FAMU-FSU College of Engineering, Florida State University (FSU), Tallahassee, Florida 32310, United States

Department of Scientific Computing, 400 Dirac Science Library, FSU, Tallahassee, Florida 32304, United States

Materials Science and Engineering Program, High Performance Materials Institute, FSU, Tallahassee, Florida 32310, United States;

Condensed Matter Theory, National High Magnetic Field Laboratory (NHMFL), FSU, Tallahassee, Florida 32310, United States

Department of Physics, The Pennsylvania State University, University Park, Pennsylvania 16802, United States

Key Laboratory of Advanced Materials (MOE), School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China

Center for 2-Dimensional and Layered Materials, The Pennsylvania State University, University Park, Pennsylvania 16802, United States

Institute of Carbon Science and Technology, Shinshu University, Wakasato 4-17-1, Nagano 380-8553, Japan

Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States

Funding

Ministry of Science and Technology of the People's Republic of China · Division of Emerging Frontiers in Research and Innovation · Army Research Office · Tsinghua University · National Natural Science Foundation of China · Beijing Nova Program

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