College of Materials Science and Engineering, State Key Laboratory of Advanced Design and Manufacturing for Vehicle Body, Hunan University, Changsha, Hunan 410082, China.
National Synchrotron Radiation Research Center, Hsinchu 300, Taiwan.
Proc Natl Acad Sci U S A. 2023 Jun 6;120(23):e2222096120. doi: 10.1073/pnas.2222096120. Epub 2023 May 30.
Rational design and synthesis of high-performance electrocatalysts for ethanol oxidation reaction (EOR) is crucial to large-scale commercialization of direct ethanol fuel cells, but it is still an incredible challenge. Herein, a unique Pd metallene/TiCT MXene (Pdene/TiCT)-supported electrocatalyst is constructed via an in-situ growth approach for high-efficiency EOR. The resulting Pdene/TiCT catalyst achieves an ultrahigh mass activity of 7.47 A mg under alkaline condition, as well as high tolerance to CO poisoning. In situ attenuated total reflection-infrared spectroscopy studies combined with density functional theory calculations reveal that the excellent EOR activity of Pdene/TiCT catalyst is attributed to the unique and stable interfaces which reduce the reaction energy barrier of *CHCO intermediate oxidation and facilitate oxidative removal of CO poisonous species by increasing the Pd-OH binding strength.
理性设计和合成高效电催化剂对于直接乙醇燃料电池的大规模商业化至关重要，但这仍然是一个巨大的挑战。在此，通过原位生长方法构建了一种独特的 Pd 金属烯/TiCT MXene（Pdene/TiCT）负载型电催化剂，用于高效乙醇氧化反应（EOR）。所得到的 Pdene/TiCT 催化剂在碱性条件下实现了超高的质量活性 7.47 A mg-1，并且对 CO 中毒具有高耐受性。原位衰减全反射-红外光谱研究结合密度泛函理论计算表明，Pdene/TiCT 催化剂具有优异的 EOR 活性，这归因于独特且稳定的界面，降低了*CHCO 中间氧化反应的能垒，并通过增加 Pd-OH 结合强度促进 CO 中毒物种的氧化去除。
