Intrinsic insight on localized surface plasmon resonance enhanced methanol electro-oxidation over a Au@AgPt hollow urchin-like nanostructure,Journal of Materials Chemistry A

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Intrinsic insight on localized surface plasmon resonance enhanced methanol electro-oxidation over a Au@AgPt hollow urchin-like nanostructure
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020/03/10 , DOI: 10.1039/c9ta13567g
Jinglei Bi _{1,

2,

3,

4,

5} , Pengfei Gao _{6,

7,

8} , Bin Wang _{1,

2,

3,

4,

5} , Xiaojing Yu _{5,

8,

9,

10} , Chuncai Kong _{1,

2,

3,

4,

5} , Liang Xu _{1,

2,

3,

4,

5} , Xiaojing Zhang _{1,

2,

3,

4,

5} , Shengchun Yang _{1,

2,

3,

4,

5}

Affiliation

The plasmon effect on the catalytic performance of metal nanoparticles (NPs) has shown great potential for the design of novel catalytic reactions. However, the intrinsic mechanisms underlying the catalysis triggered by localized surface plasmon resonance (LSPR) are still ambiguous. In this work, we construct Au@AgPt hollow urchin-like structures (Au@AgPt HUSs) with an ultra-thin Pt shell for the electrocatalytic methanol oxidation reaction (MOR) in an alkaline solution under irradiation (200 mW cm_m⁻²). A superior MOR mass activity (3.26 A mg⁻¹ Pt) is achieved on Au@AgPt HUSs, which is 5.43 times that of commercial Pt black catalysts (0.6 A mg⁻¹ Pt) under irradiation. It is also reported that localized heating, which results from the photothermal effect under irradiation, can accelerate the reaction kinetics of MOR over Au@AgPt HUSs. Theoretical calculations demonstrate that the reduced lowest unoccupied molecular orbital (LUMO) energy level of CO induced by the localized electric field can accelerate the rate-determining step *CO to *COOH, and the energetic hot carriers provide energy to promote the transfer of *CO from the hollow Pt site to the top Pt site. Thus, the hollow Pt active sites poisoned by *CO can be reactivated due to the *CO transfer mechanism, leading to more available active sites for the MOR process. This work reveals the intrinsic effect of LSPR on catalysis and paves the way to boost conventional catalytic reactions by introducing solar energy flux.

中文翻译：

关于局部表面等离子体共振的内在洞察力增强了Au @ AgPt空心顽童状纳米结构上的甲醇电氧化

等离子体对金属纳米颗粒（NPs）催化性能的影响已显示出设计新型催化反应的巨大潜力。但是，由局部表面等离振子共振（LSPR）触发的催化作用的内在机理仍然不明确。在这项工作中，我们构建的Au @ AgPt中空海胆状结构（金@ AgPt胡斯）与超薄的Pt壳照射下在碱性溶液中的电甲醇氧化反应（MOR）（200毫瓦厘米_米^-2）。Au @ AgPt HUSs具有优异的MOR质量活性（3.26 A mg ^-1 Pt），是商用Pt黑催化剂（0.6 A mg ^-1）的5.43倍Pt）照射下。也有报道称，局部加热是由辐照下的光热效应引起的，可以加速MOR在Au @ AgPt HUSs上的反应动力学。理论计算表明，局部电场引起的CO的最低最低未占据分子轨道（LUMO）能级降低，可以将速率确定步骤* CO转化为* COOH，而高能热载流子则提供能量来促进* CO的转移从空心Pt站点到顶部Pt站点。因此，由于* CO转移机制，被* CO污染的中空Pt活性位点可以重新活化，从而导致MOR过程中有更多可用的活性位点。这项工作揭示了LSPR对催化的内在作用，并通过引入太阳能通量为增强常规催化反应铺平了道路。

更新日期：2020-04-08

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