Oxygen Vacancies and Interface Engineering on Amorphous/Crystalline CrOx‐Ni3N Heterostructures toward High‐Durability and Kinetically Accelerated Water Splitting
Abstract:and long-term durability over 500 h. Our findings highlight the accelerated water-splitting performance on the oxygen-vacancy and interface modulated catalysts and shed light on the fabrication of advanced heterostructures for other catalytic reactions. Figure 7. a) The schematic illustration of the CrO x -Ni 3 N for overall water splitting. b) The performance of the CrO x -Ni 3 N//CrO x -Ni 3 N and Ni 3 N//Ni 3 N for overall water splitting, the inset image shows the comparison of the needed voltage to drive … Show more
“…Surface oxidation was also found in other HER electrocatalysts. 49,50 For Ni 3 N/Co 4 N, the Co binding energy of the Co–N bond shifts positively after HER testing (Fig. S4c and S5c†), which may arise from charge transfer of Co to the hydrogen intermediate on the catalyst.…”
“…Surface oxidation was also found in other HER electrocatalysts. 49,50 For Ni 3 N/Co 4 N, the Co binding energy of the Co–N bond shifts positively after HER testing (Fig. S4c and S5c†), which may arise from charge transfer of Co to the hydrogen intermediate on the catalyst.…”
“…DFT calculations were employed to investigate the modulation in the electronic structures resulting from the V‐doping and synergistic effect of the core and the shell materials in the amorphous‐shell@crystalline‐core heterostructures and their effect on the electrocatalytic activities for OER and HER in comparison to their crystalline‐core and amorphous shell counterparts ( Figure 8 , Figures S26–S33 , Supporting Information), similar to previous report. [ 79 ] The models representing crystalline Co 4 N and V‐doped Co 4 N core are shown in Figure S26 , Supporting Information, which reveals the significance of vanadium dopants in water adsorption. The adsorption energy of water on different doping concentrations of vanadium (V x% ‐Co 4 N, x = 1,3 and 5 at %) is found to be more favorable at the vanadium sites, as can be seen in Figure S27 , Supporting Information.…”
Section: Mechanistic Study Using Density Functional Theory (Dft)mentioning
Introducing amorphous and ultrathin nanosheets of transition bimetal phosphate arrays that are highly active in the oxygen evolution reaction (OER) as shells over an electronically modulated crystalline core with low hydrogen absorption energy for an excellent hydrogen evolution reaction (HER) can boost the sluggish kinetics of the OER and HER in alkaline electrolytes. Therefore, in this study, ultrathin and amorphous cobalt‐nickel‐phosphate (CoNiPO
x
) nanosheet arrays are deposited over vanadium (V)‐doped cobalt‐nitride (V
3%
‐Co
4
N) crystalline core nanowires to obtain amorphous‐shell@crystalline‐core mesoporous 3D‐heterostructures (CoNiPO
x
@V‐Co
4
N/NF) as bifunctional electrocatalysts. The optimized electrocatalyst shows extremely low HER and OER overpotentials of 53 and 270 mV at 10 mA cm
−2
, respectively. The CoNiPO
x
@V
3%
‐Co
4
N/NF (+/−) electrolyzer utilizing the electrocatalyst as both anode and cathode demonstrates remarkable overall water‐splitting activity, requiring a cell potential of only 1.52 V at 10 mA cm
−2
, 30 mV lower than that of the RuO
2
/NF (+)/20%‐Pt/C/NF (−) electrolyzer. Such impressive bifunctional activities can be attributed to abundant active sites, adjusted electronic structure, lower charge‐transfer resistance, enhanced electrochemically active surface area (ECSA), and surface‐ and volume‐confined electrocatalysis resulting from the synergistic effects of the crystalline V
3%
‐Co
4
N core and amorphous CoNiPO
x
shells boosting water splitting in alkaline media.
“…3d, the deconvoluted O 1s spectra present three peaks at 530.4, 531.3 and 532.4 eV, which can be assigned to the Ni-O bonds, oxygen vacancies and adsorbed oxygen species on the surface, respectively. 52,53 In comparison with NiO-LAL, all the peaks of NiO 4 -CN in Ni 2p and O 1s spectra exhibit greatly positive shis, revealing electron redistribution and interfacial interaction. The XPS results conrm that there is not only physical adsorption between g-C 3 N 4 and NiO-LAL, but also electron transfer and interfacial interaction to assemble NiO 4 -CN composites, which is an essential factor in the promotion of photocatalytic performance possibly.…”
Section: Morphology and Structure Characterizationmentioning
The interface between amorphous and crystalline plays an important role in improving the photocatalytic performance due to the optimization of both conductivity and reaction activity of active sites of cocatalysts...
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