On-purpose atomic scale design of catalytic sites, specifically active and selective at low temperature for a target reaction, is a key challenge. Here, we report teamed Pd₁ and Mo₁ single-atom sites that exhibit high activity and selectivity for anisole hydrodeoxygenation to benzene at low temperatures, 100–150 °C, where a Pd metal nanoparticle catalyst or a MoO₃ nanoparticle catalyst is individually inactive. The catalysts built from Pd₁ or Mo₁ single-atom sites alone are much less effective, although the catalyst with Pd₁ sites shows some activity but low selectivity. Similarly, less dispersed nanoparticle catalysts are much less effective. Computational studies show that the Pd₁ and Mo₁ single-atom sites activate H₂ and anisole, respectively, and their combination triggers the hydrodeoxygenation of anisole in this low-temperature range. The Co₃O₄ support is inactive for anisole hydrodeoxygenation by itself but participates in the chemistry by transferring H atoms from Pd₁ to the Mo₁ site. This finding opens an avenue for designing catalysts active for a target reaction channel such as conversion of biomass derivatives at a low temperature where neither metal nor oxide nanoparticles are.

中文翻译：

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通过配对 Pd1 和 Mo1 单原子位点开启生物质衍生物的低温催化转化


催化位点的有目的地原子尺度设计，特别是在低温下对目标反应的活性和选择性设计，是一项关键挑战。在这里，我们报告了配对的 Pd₁ 和 Mo₁ 单原子位点，它们在 100-150 °C 的低温下表现出对苯甲醚加氢脱氧的高活性和选择性，其中 Pd 金属纳米颗粒催化剂或 MoO₃ 纳米颗粒催化剂单独无活性。单独由 Pd₁ 或 Mo₁ 单原子位点构建的催化剂效果要差得多，尽管具有 Pd₁ 位点的催化剂显示出一些活性但选择性较低。同样，分散性较差的纳米颗粒催化剂的效果要差得多。计算研究表明，Pd₁ 和 Mo₁ 单原子位点分别激活 H₂ 和苯甲醚，它们的组合在此低温范围内触发苯甲醚的加氢脱氧。Co₃O₄ 负载物本身对苯甲醚加氢脱氧无活性，但通过将 H 原子从 Pd₁ 转移到 Mo₁ 位点参与化学反应。这一发现为设计对目标反应通道具有活性的催化剂开辟了一条途径，例如在金属和氧化物纳米颗粒都没有的低温下转化生物质衍生物。