Activating Glycerol Deep Oxidation via Au-TiOx Interfacial Synergy in Bimetallic Nanocatalysts

IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Yu Liu, Rong Peng, Ying Xu, Xiaoqiong Liu, Yi Song, Wenwei Liu, Wu Tianli, Junwei Zhang, Tao Li
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Abstract

Glycerol, as a renewable fuel with high energy density, has broad application prospects in green energy conversion.However, its electrocatalytic oxidation is limited by the activity and selectivity of catalysts, which severely restricts the efficient release of energy. In this work, we report a facile co-reduction synthesis of bimetallic Au-Ti nanoparticles featuring abundant Au-TiO x interfaces, which nearly doubled the mass activity for glycerol electrooxidation from 1.420 A mg Au -¹ to 2.717 A mg Au -¹, and presented an impressively high mass activity retention after the stability test. In situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) analysis confirms that Au-Ti alloy shows a deeper oxidation behaviour. Density functional theory (DFT) calculations further reveal that the formation of Au-TiO x interfaces gives rise to bifunctional synergistic sites, which facilitate the cooperative adsorption of glycerol and hydroxyl species, thereby overcoming the limitations of single-type active sites on Au/C. Meanwhile, CO adsorption further enhances the binding of hydroxyl groups, synergistically promoting deep oxidation of glycerol.
双金属纳米催化剂中Au-TiOx界面协同作用激活甘油深度氧化
甘油作为一种能量密度高的可再生燃料,在绿色能源转化中具有广阔的应用前景。但其电催化氧化受到催化剂活性和选择性的限制,严重制约了能量的有效释放。在这项工作中,我们报告了一种容易的共还原合成具有丰富Au- tio x界面的双金属Au- ti纳米颗粒,该纳米颗粒将甘油电氧化的质量活性从1.420 a mg Au-¹增加到2.717 a mg Au-¹,并且在稳定性测试后显示出令人惊讶的高质量活性保留。原位衰减全反射表面增强红外吸收光谱(ATR-SEIRAS)分析证实,Au-Ti合金表现出更深的氧化行为。密度泛函理论(DFT)计算进一步表明,Au- tio x界面的形成产生了双功能协同位点,促进了甘油和羟基的协同吸附,从而克服了Au/C上单一类型活性位点的局限性。同时,CO的吸附进一步增强了羟基的结合,协同促进甘油的深度氧化。
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来源期刊
Journal of Materials Chemistry A
Journal of Materials Chemistry A CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
19.50
自引率
5.00%
发文量
1892
审稿时长
1.5 months
期刊介绍: The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.
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