Boosting electrocatalytic water oxidation of NiFe layered double hydroxide via the synergy of 3d-4f electron interaction and citrate intercalation
Boosting electrocatalytic water oxidation of NiFe layered double hydroxide via the synergy of 3d-4f electron interaction and citrate intercalation
复制标题
通过3d-4f电子相互作用和柠檬酸盐插层的协同作用促进NiFe层状双氢氧化物的电催化水氧化
DOI：
10.1039/d2ta06801j
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发表时间：
2022-12-13
影响因子：
11.9
通讯作者：
Ma, Renzhi
中科院分区：
文献类型：
--
作者：
Chen, Shuo;Zheng, Zhicheng;Ma, Renzhi
合理的形貌设计和电子结构调制可以轻松促进NiFe层状双氢氧化物（LDH）的析氧反应（OER）。在此，通过共沉淀法合成了插层柠檬酸根阴离子的多级三金属NiFeCe-LDH。具有丰富活性位点的自支撑多孔 LDH 纳米片 (PN) 具有强大的结构稳定性，而插入的柠檬酸盐和 Ce 离子的引入通过 3d-4f 电子相互作用调节电子结构优化了本征活性。结果，优化的Ni:Fe:Ce摩尔比为2:0.7:0.3的PNs表现出最佳的OER活性，在仅224 mV的过电势下提供20 mA cm(-2)，塔菲尔斜率为54.0 mV dec(-1)，并在100 mA cm(-2)的高电流密度下表现出类似于160 h的优异耐久性。实验和理论研究进一步证实了强烈的3d-4f电子相互作用，显着提高了含氧中间体的吸附/解吸性能。这项工作提供了通过3d-4f电子相互作用和适当阴离子组成的合理协同作用来开发高性能电催化剂的策略。
Rational morphology design and electronic structure modulation can facilely boost the oxygen evolution reaction (OER) of NiFe layered double hydroxides (LDHs). Herein, hierarchical trimetallic NiFeCe-LDH intercalated with citrate anions was synthesized via a co-precipitation method. The self-supported porous LDH nanosheets (PNs) with abundant active sites exposed contributed to robust structural stability while the intercalated citrate and the introduction of Ce ions optimized intrinsic activity by modulating the electronic structure through 3d-4f electron interaction. As a result, PNs with an optimized Ni : Fe : Ce molar ratio of 2 : 0.7 : 0.3 exhibited the best OER activity of delivering 20 mA cm(-2) at an overpotential of only 224 mV with a Tafel slope of 54.0 mV dec(-1) and excellent durability of similar to 160 h at a high current density of 100 mA cm(-2). Experimental and theoretical investigations further confirmed the strong 3d-4f electron interaction, dramatically improving the adsorption/desorption properties of the oxygen-containing intermediates. This work provides a strategy to develop high-performance electrocatalysts through the rational synergism of 3d-4f electron interaction and appropriate anion composition.