Edge-Sharing Octahedrally Coordinated NiFe Dual Active Sites on ZnFe(2) O(4) for Photoelectrochemical Water Oxidation.
Edge-Sharing Octahedrally Coordinated NiFe Dual Active Sites on ZnFe(2) O(4) for Photoelectrochemical Water Oxidation.
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DOI：
10.1002/advs.202301869
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发表时间：
2023-08
期刊：
影响因子：
15.1
通讯作者：
Bao, Jun
中科院分区：
文献类型：
--
作者：
Jiang, Zhiyong;Zhu, Xiaodi;Wang, Zhiyu;Liu, Wei;Yan, Wensheng;Sivula, Kevin;Bao, Jun
尖晶石氧化物（AB 2 O 4）中八面体位置（BOh）的结构特性在氧相关反应的电化学性能中起着至关重要的作用。然而，由于其晶体结构的复杂性，AB 2 O 4的精确操作仍然具有挑战性。在这里，报道了一种简单而通用的熔盐介导的策略，在铁酸锌（ZnFe 2 O 4，ZFO）表面的Boh位点中有意引入Ni 2+，以促进光电化学（PEC）水裂解的活性位点。与裸ZFO相比，所产生的光阳极（ZFO-MSNi）显示出1.450 mV的显著阴极偏移（开启电压为1.00.6 VRHE）以及在1.23 VRHE下PEC水氧化的1倍太阳光电流密度。全面的结构表征清楚地揭示了ZFO-MSNi中引入的Ni 2+的局部结构。观察到更少的表面捕获态，而精确引入的Ni 2+和相关的相邻Fe（3-σ）+（0<σ<1）位点以共边八面体构型结合，以用作PEC水氧化的Ni-Fe双活性位点。此外，开路电位测量和快速扫描伏安法研究进一步深入了解了增强的PEC性能。总的来说，这项工作显示了一个通用的策略，以调节光电极的表面活性位点，以提高PEC太阳能转换系统的性能。通过一种简单的熔盐介导策略，在ZnFe 2 O 4光阳极表面精确构建了共边八面体配位的Ni 2 +-Fe（3-σ）+（0<σ<1）双活性位，具有较少的捕获态.光电化学水氧化过程中，光电流起始电位发生了约450 mV的显着阴极位移，1太阳光电流密度明显增强。
The structural properties of octahedral sites (BOh) in spinel oxides (AB2O4) play vital roles in the electrochemical performance of oxygen‐related reactions. However, the precise manipulation of AB2O4 remains challenging due to the complexity of their crystal structure. Here, a simple and versatile molten‐salt‐mediated strategy is reported to introduce Ni2+ in Boh sites intentionally on the surface of zinc ferrite (ZnFe2O4, ZFO) to promote the active sites for photoelectrochemical (PEC) water splitting. The as‐created photoanode (ZFO‐MSNi) shows a remarkable cathodic shift of ≈ 450 mV (turn‐on voltage of ≈ 0.6 VRHE) as well as three times the 1‐sun photocurrent density at 1.23 VRHE for PEC water oxidation in comparison with bare ZFO. A comprehensive structural characterization clearly reveals the local structure of the introduced Ni2+ in ZFO‐MSNi. Fewer surface trapping states are observed while the precisely introduced Ni2+ and associated neighboring Fe(3‐σ)+ (0<σ<1) sites unite in an edge‐sharing octahedral configuration to function as Ni—Fe dual active sites for PEC water oxidation. Moreover, open circuit potential measurements and rapid‐scan voltammetry investigation give further insight into the enhanced PEC performance. Overall, this work displays a versatile strategy to regulate the surface active sites of photoelectrodes for increasing performance in PEC solar energy conversion systems. Edge‐sharing octahedrally coordinated Ni2+—Fe(3‐σ)+ (0<σ<1) dual active sites are precisely constructed on the surface of ZnFe2O4 photoanodes with fewer trapping states through a simple molten‐salt‐mediated strategy. A remarkable cathodic shift of ≈ 450 mV with photocurrent onset potential as well as obviously enhanced 1‐sun photocurrent density is achieved for photoelectrochemical water oxidation.
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