Huang Xiaoxiao, He Zhi-Long, Chen Yangpeng, Xu Qiyan, Zhu Mingshan, Zhai Chunyang
School of Materials Science and Chemical Engineering, Ningbo University, Ningbo 315211, PR China.
School of Metallurgical Engineering, Anhui University of Technology, Manshan 243032, PR China.
J Colloid Interface Sci. 2022 Nov;625:850-858. doi: 10.1016/j.jcis.2022.06.108. Epub 2022 Jun 24.
Precise design of high efficacious catalysts and the insight into the mechanism for photo-electrocoupling catalytic methanol oxidation reaction (MOR) are two major issues for the development and practical application of direct methanol fuel cells (DMFCs). Herein, a novel self-standing three-dimensional nanosheet assembly PdAu nanoflower with local surface plasmon resonance effect is fabricated to acquire excellent catalytic performance and explore the photo-electrocatalytic mechanism for MOR. Interestingly, the PdAu nanoflower electrocatalyst exhibits superior mass activity than pure Pd and Pd/C catalysts thanks to the abundant active sites and efficacious charge transfer. Further on, with the assistance of LSPR effect, the catalytic activity for MOR of PdAu catalyst (4179.04 mA mg) under visible light illumination achieved 2.41-fold than dark conditions (1731.42 mA mg). Moreover, the long-term durability of PdAu catalysts with visible light is also improved compare to dark condition and other mentioned Pd catalyst. More significantly, a photo-electrocoupling CO-free dominant mechanism is proposed to in-depth understand the promotion of catalytic activity and durability for MOR. This contribution provides the rational design of plasma-enhanced high-effective photo-electrocatalyst and reveals a CO-free dominant MOR mechanism for the progress of future liquid direct fuel cells.
精确设计高效催化剂以及深入了解光电耦合催化甲醇氧化反应（MOR）的机理是直接甲醇燃料电池（DMFC）发展和实际应用的两个主要问题。在此，制备了一种具有局域表面等离子体共振效应的新型自立式三维纳米片组装PdAu纳米花，以获得优异的催化性能并探索MOR的光电催化机理。有趣的是，由于丰富的活性位点和有效的电荷转移，PdAu纳米花电催化剂表现出比纯Pd和Pd/C催化剂更高的质量活性。进一步地，在LSPR效应的辅助下，PdAu催化剂在可见光照射下对MOR的催化活性（4179.04 mA mg）比黑暗条件下（1731.42 mA mg）提高了2.41倍。此外，与黑暗条件和其他提及的Pd催化剂相比，PdAu催化剂在可见光下的长期耐久性也得到了提高。更重要的是，提出了一种无CO的光电耦合主导机制，以深入了解对MOR催化活性和耐久性的促进作用。这一贡献为等离子体增强高效光电催化剂的合理设计提供了依据，并揭示了一种无CO主导的MOR机制，以推动未来液体直接燃料电池的发展。
