<br>异质结诱导的 Ni3+/Ni2+ 位点快速转变可介导尿素氧化以实现节能制氢,Advanced Materials

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异质结诱导的 Ni3+/Ni2+ 位点快速转变可介导尿素氧化以实现节能制氢
Advanced Materials ( IF 27.4 ) Pub Date : 2024-01-16 , DOI: 10.1002/adma.202311766
Peng Guo _{1,

2} , Shoufu Cao ₃ , Wenjing Huang ₄ , Xiaoqing Lu ₃ , Weizhe Chen _{1,

2} , Youzi Zhang _{1,

2} , Yijin Wang _{1,

2} , Xu Xin _{1,

2} , Ruiqing Zou _{1,

2} , Sibi Liu _{1,

2} , Xuanhua Li _{1,

2}

Affiliation

水电解是一种环保的制氢策略，但能耗很高。采用镍基电催化剂代替理论电压较低的尿素氧化反应(UOR)来代替水氧化反应，可以降低制氢能耗。主要障碍仍然是传统Ni ³⁺催化途径中积累的Ni ³⁺和*COO之间的强相互作用。在此，通过构建偏磷酸镍和碲化镍的异质结（Ni ₂ P ₄ O ₁₂ /NiTe），一种新的Ni ³⁺ /Ni ²⁺介导的UOR途径，有效降低了UOR的能垒并避免了Ni的积累开发了电催化剂上的³⁺和*COO 的过度吸附。因此，Ni ₂ P ₄ O ₁₂ /NiTe表现出1.313 V的极低电势，可实现10 mA cm ^-2的电流密度，从而实现有效的尿素氧化反应，同时在10 mA cm -2 下表现出仅24 mV的过电势^{- 2}用于析氢反应。在两侧使用Ni ₂ P ₄ O ₁₂ /NiTe构建的尿素电解电解槽在1.475 V的低电池电压下达到100 mA cm ^{-2 ，}并且在500小时内具有优异的稳定性以及接近100%的法拉第效率。

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Heterojunction-Induced Rapid Transformation of Ni3+/Ni2+ Sites which Mediates Urea Oxidation for Energy-Efficient Hydrogen Production

Water electrolysis is an environmentally-friendly strategy for hydrogen production but suffers from significant energy consumption. Substituting urea oxidation reaction (UOR) with lower theoretical voltage for water oxidation reaction adopting nickel-based electrocatalysts engenders reduced energy consumption for hydrogen production. The main obstacle remains strong interaction between accumulated Ni³⁺ and *COO in the conventional Ni³⁺-catalyzing pathway. Herein, a novel Ni³⁺/Ni²⁺ mediated pathway for UOR via constructing a heterojunction of nickel metaphosphate and nickel telluride (Ni₂P₄O₁₂/NiTe), which efficiently lowers the energy barrier of UOR and avoids the accumulation of Ni³⁺ and excessive adsorption of *COO on the electrocatalysts, is developed. As a result, Ni₂P₄O₁₂/NiTe demonstrates an exceptionally low potential of 1.313 V to achieve a current density of 10 mA cm⁻² toward efficient urea oxidation reaction while simultaneously showcases an overpotential of merely 24 mV at 10 mA cm⁻² for hydrogen evolution reaction. Constructing urea electrolysis electrolyzer using Ni₂P₄O₁₂/NiTe at both sides attains 100 mA cm⁻² at a low cell voltage of 1.475 V along with excellent stability over 500 h accompanied with nearly 100% Faradic efficiency.

更新日期：2024-01-16

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