TY - JOUR
T1 - Tunable d-Band Centers of Ni5P4 Ultra-Thin Nanosheets for Highly-Efficient Hydrogen Evolution Reaction
AU - Miao, Chengcheng
AU - Zang, Yanmei
AU - Wang, Hang
AU - Zhuang, Xinming
AU - Han, Ning
AU - Yin, Yanxue
AU - Ma, Yandong
AU - Chen, Ming
AU - Dai, Ying
AU - Yip, Sen Po
AU - Ho, Johnny C.
AU - Yang, Zai xing
N1 - Funding Information:
C.M., Y.Z., H.W., and X.Z. contributed equally to this work. The authors acknowledge the National Natural Science Foundation of China (No. 61904096), Taishan Scholars Program of Shandong Province (No. tsqn201812006), Shandong University Multidisciplinary Research and Innovation Team of Young Scholars (No. 2020QNQT015), “Outstanding Youth Scholar and Qilu Young Scholar” programs of Shandong University, and the Environment and Conservation Fund of Hong Kong SAR, China (No. ECF 2020‐13).
Publisher Copyright:
© 2022 Wiley-VCH GmbH.
PY - 2022/8/3
Y1 - 2022/8/3
N2 - Although the recent advance of ultra-thin 2D nanosheets for hydrogen evolution reaction (HER) is remarkable, there are still substantial challenges to reliably control their physioelectric and electrochemical properties to employ as highly-efficient electrocatalysts. Herein, based on complementary theoretical and experimental studies, the d-band center position of ultra-thin 2D Ni5P4 nanosheets can be manipulated by simple heteroatom doping. Interestingly, the Fe-doped nanosheets yield the lowest d-band center position, but they do not display the optimal Gibbs free energy of adsorbed H atoms due to the imbalance of adsorption and desorption of adsorbed H atoms. With the proper Co doping (i.e., 20%), the nanosheets exhibit the best electrocatalytic performance along with an excellent stability. The overpotential is only 100.5 mV at 10 mA cm−2 with a Tafel slope of 65.8 mV dec−1, which is superior than those of Fe-doped, Cu-doped, and pristine Ni5P4 nanosheets. Ultraviolet photoelectron and X-ray photoelectron spectroscopy further verify the downshift of d-band centers of nanosheets by optimal doping, illustrating that Ni with the lower binding energy mainly dominates the active sites. All these results provide a valuable design scheme of dopants to control the d-band center position of nanosheets for next-generation highly-efficient HER electrocatalysts.
AB - Although the recent advance of ultra-thin 2D nanosheets for hydrogen evolution reaction (HER) is remarkable, there are still substantial challenges to reliably control their physioelectric and electrochemical properties to employ as highly-efficient electrocatalysts. Herein, based on complementary theoretical and experimental studies, the d-band center position of ultra-thin 2D Ni5P4 nanosheets can be manipulated by simple heteroatom doping. Interestingly, the Fe-doped nanosheets yield the lowest d-band center position, but they do not display the optimal Gibbs free energy of adsorbed H atoms due to the imbalance of adsorption and desorption of adsorbed H atoms. With the proper Co doping (i.e., 20%), the nanosheets exhibit the best electrocatalytic performance along with an excellent stability. The overpotential is only 100.5 mV at 10 mA cm−2 with a Tafel slope of 65.8 mV dec−1, which is superior than those of Fe-doped, Cu-doped, and pristine Ni5P4 nanosheets. Ultraviolet photoelectron and X-ray photoelectron spectroscopy further verify the downshift of d-band centers of nanosheets by optimal doping, illustrating that Ni with the lower binding energy mainly dominates the active sites. All these results provide a valuable design scheme of dopants to control the d-band center position of nanosheets for next-generation highly-efficient HER electrocatalysts.
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U2 - 10.1002/admi.202200739
DO - 10.1002/admi.202200739
M3 - Article
AN - SCOPUS:85135532547
SN - 2196-7350
VL - 9
JO - Advanced Materials Interfaces
JF - Advanced Materials Interfaces
IS - 22
M1 - 2200739
ER -