Two-Dimensional Siloxene as an Advanced Support of Platinum for Superior Hydrogen Evolution and Methanol Oxidation Electrocatalysis
Two-Dimensional Siloxene as an Advanced Support of Platinum for Superior Hydrogen Evolution and Methanol Oxidation Electrocatalysis
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DOI：
10.1016/j.mtphys.2022.100931
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发表时间：
2022-11
影响因子：
11.5
通讯作者：
Qinqin Chen;Cuicui Du;Yixin Yang;Qin-yin Shen;Junfeng Qin;Min Hong;Xiaohua Zhang;Jinhua Chen-Jinhua
中科院分区：
文献类型：
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作者：
Qinqin Chen;Cuicui Du;Yixin Yang;Qin-yin Shen;Junfeng Qin;Min Hong;Xiaohua Zhang;Jinhua Chen-Jinhua
为了提高多用途铂在电化学能量转换中的利用效率，精确选择载体材料是一种非常有前途的策略。在这里，我们展示了新型的二维硅氧烯作为铂的高级载体，基于不寻常的金属-载体相互作用，在增强双功能电催化放氢(HER)和甲醇氧化(MOR)方面的竞争优势。采用简单的湿化学法在有机硅薄膜上负载铂纳米粒子，成功地制备了铂纳米粒子/有机硅电催化剂。与商用铂碳(20wt%)相比，超低铂含量(1.3wt%)的铂纳米粒子/硅氧烷在酸性介质中对HER和MOR具有良好的电催化活性和良好的稳定性。对于她来说，需要24 mV的小过电位来驱动10 mA/cm−2电流，同时具有低塔菲尔斜率(24.6mV/12−1)。同时，获得了1957 mA/mg−-1的优秀铂质量活度，是铂/碳的12.6倍。理论计算表明，结合能的优化有利于HER和MOR电催化过程中相关吸附物的脱附或吸附，从而提高了铂的利用效率。特别是，这种支撑工程可以触发从铂到硅氧烯的氢溢出，促进氢气的生成，这归因于一种独特的基于氢溢出的HER途径，该途径具有良好的质子在铂位上的吸附和从硅氧烯上高效的氢解吸。
To improve the utilization efficiency of versatile platinum (Pt) in electrochemical energy conversion, precisely choosing support materials is a significantly promising strategy. Herein, we demonstrate the competitive advantages of novel two-dimensional Siloxene as the advanced support of Pt toward enhancing bifunctional electrocatalysis for hydrogen evolution (HER) and methanol oxidation (MOR) based on unusual metal–support interactions. The Pt NPs/Siloxene electrocatalyst by supporting Pt nanoparticles on Siloxene sheets is successfully synthesized via simple wet-chemical method. Compared to commercial Pt/C (20 wt%), Pt NPs/Siloxene with ultra-low Pt content (1.3 wt%) exhibits superior electrocatalytic activity with good stability toward HER and MOR in acidic media. For HER, a small overpotential of 24 mV is required to drive 10 mA cm−2current with a low Tafel slope (24.6 mV dec−1). Meanwhile, preeminent Pt mass activity of 1957 mA mg−1for MOR is achieved, which is 12.6 times higher than that of Pt/C. Theoretical calculations indicate that the binding energies are optimized to facilitate desorption or adsorption of related adsorbates during HER and MOR electrocatalysis, and thus enhancing Pt utilization efficiency. Specially, this support engineering can trigger hydrogen spillover from Pt to Siloxene to promote hydrogen generation, attributed to a unique hydrogen spillover-based HER pathway with favorable proton adsorption on Pt sites and efficient hydrogen desorption from Siloxene.