Atomically Dispersed Ni/α-MoC Catalyst for Hydrogen Production from Methanol/Water

Lili Lin; Qiaolin Yu; Mi Peng; Aowen Li; Siyu Yao; Shuheng Tian; Xi Liu; Ang Li; Zheng Jiang; Rui Gao; Xiaodong Han; Yong-Wang Li; Xiao-Dong Wen; Wu Zhou; Ding Ma

doi:10.1021/jacs.0c10776

Atomically Dispersed Ni/α-MoC Catalyst for Hydrogen Production from Methanol/Water

J Am Chem Soc. 2021 Jan 13;143(1):309-317. doi: 10.1021/jacs.0c10776. Epub 2020 Dec 28.

Authors

Lili Lin^{1

2}, Qiaolin Yu¹, Mi Peng¹, Aowen Li³, Siyu Yao¹, Shuheng Tian¹, Xi Liu⁴, Ang Li⁵, Zheng Jiang⁶, Rui Gao^{7

8

9}, Xiaodong Han⁵, Yong-Wang Li^{7

8}, Xiao-Dong Wen^{7

8}, Wu Zhou^{3

10}, Ding Ma¹

Affiliations

¹ Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering and College of Engineering, and BIC-ESAT, Peking University, Beijing 100871, China.
² Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, China.
³ School of Physical Sciences and CAS Key Laboratory of Vacuum Physics, University of Chinese Academy of Sciences, Beijing 100049, China.
⁴ School of Chemistry and Chemical, In-situ Center for Physical Science, Shanghai Jiao Tong University, Shanghai 200240, China.
⁵ Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing 100024, China.
⁶ Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China.
⁷ State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China.
⁸ National Energy Center for Coal to Liquids, Synfuels China Company Limited, Beijing 101400, China.
⁹ School of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021, China.
¹⁰ CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing 100049, China.

PMID: 33369393
DOI: 10.1021/jacs.0c10776

Abstract

Methanol-water reforming is a promising solution for H₂ production/transportation in stationary and mobile hydrogen applications. Developing inexpensive catalysts with sufficiently high activity, selectivity, and stability remains challenging. In this paper, nickel-supported over face-centered cubic (fcc) phase α-MoC has been discovered to exhibit extraordinary hydrogen production activity in the aqueous-phase methanol reforming reaction. Under optimized condition, the hydrogen production rate of 2% Ni/α-MoC is about 6 times higher than that of conventional noble metal 2% Pt/Al₂O₃ catalyst. We demonstrate that Ni is atomically dispersed over α-MoC via carbon bridge bonds, forming a Ni₁-C_x motif on the carbide surface. Such Ni₁-C_x motifs can effectively stabilize the isolated Ni₁ sites over the α-MoC substrate, rendering maximized active site density and high structural stability. In addition, the synergy between Ni₁-C_x motif and α-MoC produces an active interfacial structure for water dissociation, methanol activation, and successive reforming processes with compatible activity.