过渡金属调节酸性位点促进钯催化剂C-H键裂解能力提高甲烷完全燃烧性能Regulating acid sites by transition metals to promote C-H bond cracking ability of Pd catalysts for methane complete combustion performance improvement
夏良辉,王晶晶,建艳飞,刘昱洁,何炽
摘要(Abstract):
甲烷作为主要大气污染物之一,因其具有稳定的四面体分子结构,给其在温和条件下的催化氧化消除带来巨大挑战。旨在通过引入过渡金属(Cr、Mo、W)改性Pd基催化剂的酸性位点,促进C-H键的裂解,以增强甲烷催化氧化性能。通过XRD、Raman、H_2-TPR、NH_3-TPD等多种表征手段对催化剂的氧空位、酸性及氧化还原性能进行了系统探究。结果表明:过渡金属改性使得Pd催化剂的酸性位点显著增加,且过渡金属改性的PdM催化剂具有更高的氧空位数量;Mo改性的PdMo催化剂表现出更优异的氧化还原性能,而Cr和W改性的PdCr及PdW催化剂的氧化还原性能稍有下降;甲烷氧化反应结果表明,酸性位点适中的PdMo催化剂具有最优异的甲烷氧化性能,其T90温度较Pd催化剂降低约150℃,且表现出更好的反应稳定性;然而,酸性位点数量较多或较少的PdCr及PdW催化剂表现出较低的甲烷氧化活性,说明催化剂的酸性位点数量和氧化还原性能共同决定了其甲烷氧化性能。该结论为设计制备用于甲烷完全氧化的低温高效催化剂提供了思路。
关键词(KeyWords): 甲烷;钯催化剂;过渡金属;酸性位点;氧化还原性能
基金项目(Foundation): 国家重点研发计划(2022YFB4101500);; 国家自然科学基金项目(22276145,21922606) ~~
作者(Author): 夏良辉,王晶晶,建艳飞,刘昱洁,何炽
DOI: 10.19666/j.rlfd.202402036
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