期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 9, 期 4, 页码 1920-1931出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.0c08543
关键词
Metal-organic frameworks; Semi-MOF derivatives; Nickel sulfide nanoparticles; Bifunctional electrocatalysts; Water electrolysis
资金
- National Natural Science Foundation of China [21773024]
- Sichuan Science and Technology Program [2020YJ0324, 2020YJ0262]
- China Postdoctoral Science Foundation [2019M663469]
- Reformation and Development Funds for Local Region Universities from China Government in 2020 [ZCKJ 2020-11]
Electrocatalytic water splitting using nickel and nickel sulfide heteronanoparticle-embedded semi-MOFs prepared through partial sulfurization shows exceptional bifunctional activity with low overpotentials for both OER and HER. The unique nanoarchitecture of Ni-M@C-130 contributes to its outstanding catalytic performance, attributed to the combined benefits of MOF nanosheets, synergistic interactions, and improved electrical conductivity and mechanical stability. This study highlights the advantages of partial sulfurization in achieving electrochemically active heteronanoparticles within MOF nanosheets for improved bifunctional activity.
Electrocatalytic water splitting is an emerging technique to produce sustainable hydrogen energy. However, it is still challengeable to fabricate a stable, efficient, and cost-effective electrocatalyst that can overcome the sluggish reaction kinetics of water electrolysis. In order to reduce the energy barrier, for the first time, metal-organic framework (MOF)-derived nickel (Ni) and nickel sulfide (NiS) heteronanoparticle-embedded semi-MOFs are prepared by a partial sulfurization strategy. These semi-MOF electrocatalysts inherit the advantages associated with MOF architecture and nanoparticles, unlike the traditional OER catalysts such as pristine MOFs or completely pyrolyzed MOFs. Due to the unique nanoarchitecture fabricated by Ni/NiS heteronanoparticles within semi-MOF nanosheets and a carbon nanotube (CNT) network (Ni-M@C-130), it displays exceptional bifunctional activity over the other transition metal-based electrocatalysts ever reported. It requires very small overpotentials for both oxygen evolution reaction (OER; eta(10) = 244 mV) and hydrogen evolution reaction (HER; eta(10) = 123 mV), with low Tafel slopes of 47.2 and 50.8 mV/dec, respectively. Furthermore, it exhibits overpotential as low as 1.565 V (eta(10)) on nickel foam (1 mg/cm(2)) substrates for overall water splitting. The outstanding catalytic performance of Ni-M@C-130 is attributed to the combined benefits of MOF nanosheets, synergistic interactions, and improved electrical conductivity and mechanical stability. This study describes the advantages of partial sulfurization of CNT-integrated MOFs in attaining electrochemically active heteronanoparticles within MOF nanosheets to accomplish improved bifunctional activity.
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