The capability to actively control chemical reactions has enormous implications for energy generation and conversion. By integrating theory and experiments, we achieved an in-situ regulation of formic acid oxidation on a Pt (1 1 1) surface via externally applied strains. The first-principles theory predicted that compressive strains can lower the reaction overpotential to boost the formate pathway and alleviate CO poisoning on the Pt surface, while tensile strains should have the opposite effects. The experimental observations confirmed the theoretical predictions. Compressive elastic strains (approximately -0.4%) could create over 75 mV overpotential decrease, far beyond what was achieved in previous works. A mass activity (~700 mA/mg) of Pt was achieved in a broad potential range of 0.4–0.85 V (vs RHE) under compressive strains. There was no evident activity loss during the chronoamperometry test at 0.6 V. The first-principles theory, controlled synthesis and in-situ measurements were combined to achieve active control, which represents important progress in tuning the electrocatalytic activity of formic acid oxidation.

主动控制化学反应的能力对能量的产生和转化有着巨大的影响。通过整合理论和实验，我们通过外部施加的应变实现了Pt（1 1 1）表面上甲酸氧化的原位调节。第一性原理理论认为，压缩应变可以降低反应的超电势，从而促进甲酸途径并减轻Pt表面的CO中毒，而拉伸应变则具有相反的作用。实验观察证实了理论预测。压缩弹性应变（大约-0.4％）可能会导致超过75 mV的超电势下降，远远超出了先前的工作。在压缩应变下，Pt在0.4-0.85 V（vs RHE）的宽电位范围内实现了质量活性（〜700 mA / mg）。结合现场测量以实现主动控制，这在调节甲酸氧化的电催化活性方面代表了重要的进展。