关键词: Doping Hybridization orbital Intercalation Overall water splitting Re-stacking V(2)C-MXene

来  源:   DOI:10.1016/j.jcis.2024.07.025

Abstract:
Nowadays, the inherent re-stacking nature and weak d-p hybridization orbital interactions within MXene remains significant challenges in the field of electrocatalytic water splitting, leading to unsatisfactory electrocatalytic activity and cycling stability. Herein, this work aims to address these challenges and improve electrocatalytic performance by utilizing cobalt nanoparticles intercalation coupled with enhanced π-donation effect. Specifically, cobalt nanoparticles are integrated into V2C MXene nanosheets to mitigate the re-stacking issue. Meanwhile, a notable charge redistribution from cobalt to vanadium elevates orbital levels, reduces π*-antibonding orbital occupancy and alleviates Jahn-Teller distortion. Doping with tellurium induces localized electric field rearrangement resulting from the changes in electron cloud density. As a result, Co-V2C MXene-Te acquires desirable activity for hydrogen evolution reaction and oxygen evolution reaction with the overpotential of 80.8 mV and 287.7 mV, respectively, at the current density of -10 mA cm-2 and 10 mA cm-2. The overall water splitting device achieves an impressive low cell voltage requirement of 1.51 V to obtain 10 mA cm-2. Overall, this work could offer a promising solution when facing the re-stacking issue and weak d-p hybridization orbital interactions of MXene, furnishing a high-performance electrocatalyst with favorable electrocatalytic activity and cycling stability.
摘要:
如今,MXene内部固有的重堆叠性质和弱的d-p杂化轨道相互作用仍然是电催化水分解领域的重大挑战,导致不令人满意的电催化活性和循环稳定性。在这里,这项工作旨在解决这些挑战,提高电催化性能,利用钴纳米粒子插层和增强π-捐赠效应。具体来说,钴纳米粒子被整合到V2CMXene纳米片中以减轻重新堆叠问题。同时,从钴到钒的显着电荷重新分布提高了轨道水平,减少π*-反键轨道占用,减轻Jahn-Teller失真。碲掺杂会引起由于电子云密度变化而引起的局部电场重排。因此,Co-V2CMXene-Te在80.8mV和287.7mV的超电势下获得了理想的析氢反应和析氧反应活性,分别,在-10mAcm-2和10mAcm-2的电流密度下。整个水分解装置实现了令人印象深刻的1.51V的低电池电压要求,以获得10mAcm-2。总的来说,当面对MXene的重新堆叠问题和弱的d-p杂化轨道相互作用时,这项工作可以提供一个有希望的解决方案,提供具有良好电催化活性和循环稳定性的高性能电催化剂。
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