PdO is known to efficiently catalyze the oxidation of methane but suffers tremendously from sulfur poisoning that lowers its catalytic activity. In this paper, dispersion-corrected density functional theory based first principles calculations were performed to systematically screen the metal impurities M (where M is a transition metal) on a Pd1−xMxO catalyst that promote the desired adsorption energies for CH4 and SO2 to gain insights into the design of sulfation-resistant PdO-based methane oxidation catalysts. Specific Pd1−xMxO(101) catalyst was identified to thermodynamically avoid surface sulfation while maintaining the active sites for methane activation at typical experimental conditions. Results indicate a potential route of tuning the catalytic property of PdO by the introduction of a surface metal impurity.

中文翻译：

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CH4 和 SO2 在无支撑 Pd1−xMxO(101) 表面的吸附

众所周知，PdO 可以有效地催化甲烷氧化，但由于硫中毒会降低其催化活性。在本文中，进行了基于第一性原理计算的色散校正密度泛函理论，以系统地筛选 Pd1-xMxO 催化剂上的金属杂质 M（其中 M 是过渡金属），以促进 CH4 和 SO2 所需的吸附能，以获得洞察力设计耐硫酸化的 PdO 基甲烷氧化催化剂。特定的 Pd1-xMxO(101) 催化剂被确定为在热力学上避免表面硫酸化，同时在典型的实验条件下保持甲烷活化的活性位点。结果表明通过引入表面金属杂质来调节 PdO 催化性能的潜在途径。