首页|氧气电还原合成H2O2高性能电催化剂的先进设计策略

氧气电还原合成H2O2高性能电催化剂的先进设计策略

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过氧化氢(H2O2)作为环境、化工和能源领域中重要的化工原料,被广泛应用于高级氧化过程、有机化学合成及能源转化技术中。相比于传统的蒽醌法,基于氧气电还原合成H2O2技术(ORR)提供了一种经济、高效、无害的替代工艺,具备低碳生产及储能潜力。为进一步提高反应选择性及能量转化效率,开发具有高活性、高选择性和长效稳定性的电催化剂是调控反应决速步骤的中间体吸脱附行为,改善反应物种高效界面能质传递的关键,从而进一步提高ORR合成H2O2的催化活性及能量转化效率。基于此,本文系统性地综述了近年来通过ORR合成H2O2体系中高性能电催化剂的通用设计策略,从电子结构调控、几何结构调控、表面功能化修饰及原子级活性位点设计等4个方面对先进电催化剂的合成策略及调控机制进行了总结与梳理。最后,本文围绕ORR电催化剂的设计方向及应用前景提出了相应的展望与建议。
Advanced Design Strategies for High-Performance Electrocatalysts Based on Oxygen Reduction Reaction towards H2O2 Synthesis
Hydrogen peroxide(H2O2),as an important chemical raw material in the fields of environment,chemical,and energy,has become an emerging candidate in promoting energy transformation and green development of the chemical industry due to its characteristics of green environmental protection and strong sustainability.At present,over 95%of H2O2 worldwide is synthesized through the anthraquinone oxidation(AO process),which mainly involves the hydrogenation and oxidation process of anthraquinone molecules in Ni or Pd catalysts and organic solvents.However,the AO process also brings in additional costs and poses risks such as flammability and explosion during transportation,high energy consumption,and waste generation.Oxygen reduction reaction(ORR)towards H2O2 synthesis provides an economical,efficient,and harmless alternative process for the in-situ synthesis of green reagents under mild conditions.However,ORR towards H2O2 synthesis mainly faces two major challenges:low reaction selectivity and slow reaction kinetics,which lead to generally low H2O2 yield and Faraday efficiency,hindering further industrial applications.As the core of electrocatalytic reactions,the surface physicochemical properties of electrocatalysts are usually closely related to the catalytic process,directly affecting the adsorption and desorption of reaction species,thereby further affecting the overall reaction thermodynamics and kinetics.Therefore,developing electrocatalysts with high activity,high selectivity,and good stability,is the key to further improving the catalytic activity and energy conversion efficiency.Based on this,this review systematically summarizes the advanced design strategies of high-performance electrocatalysts in the H2O2 synthesis through ORR in recent years.The synthesis strategies and control mechanisms of advanced electrocatalysts are summarized and sorted out from four aspects:electronic structure control,geometric structure control,surface morphology control,and atomization active site design.Prospects and suggestions are also proposed for the design direction and application prospects of ORR electrocatalysts,which are beneficial for achieving precise control of intermediate adsorption and desorption behavior in reaction rate-determining steps,and constructing interface conditions for efficient energy and mass transfer of reaction species.

oxygen reduction reactionhydrogen peroxideelectronic structure regulationgeometric structure regulationsurface functionalization modification

丁雅妮、周伟、高继慧

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哈尔滨工业大学 能源科学与工程学院 哈尔滨 150001

氧气还原反应 过氧化氢 电子结构调控 几何结构调控 表面功能化修饰

2024

化学进展
中国科学院基础科学局,化学部,文献情报中心 国家自然科学基金委员会化学科学部

化学进展

CSTPCD北大核心
影响因子:1.079
ISSN:1005-281X
年,卷(期):2024.36(10)