Direct CO hydrogenation to higher alcohols (HA) is a promising route for high-value utilization of waste CO, but developing active and stable catalysts remains a grand challenge. For this reaction, constructing multifunctional interfaces as active sites is required to fulfill controllable C-C coupling of alkyl and CO*/CHO* species. Herein, we report a PdFe catalyst with abundant PdFe alloy-FeC interfaces via a PdFe alloy induced FeO carbidization process, which can achieve HA yield of 86.5 mg g h with 26.5% selectivity at 300 ºC, 5 MPa, and 6000 mL g h. The accelerated deactivation test unveils the PdFe catalyst exhibits better durability than the widely studied CuFe based catalysts against harsh conditions. Multiple in-situ characterization results unveil a synergetic mechanism for HA synthesis at the PdFe alloy-FeC interfaces, where PdFe alloy is responsible for CO formation and non-dissociative activation, while FeC phase promotes CO dissociation and chain propagation.

中文翻译：

---

PdFe 合金-Fe5C2 界面可有效地将 CO2 加氢为高级醇

CO直接加氢生成高级醇（HA）是废二氧化碳高价值利用的一条有前途的途径，但开发活性和稳定的催化剂仍然是一个巨大的挑战。对于该反应，需要构建多功能界面作为活性位点来实现烷基和CO*/CHO*物质的可控CC偶联。在此，我们报道了一种通过 PdFe 合金诱导 Fe3O 碳化工艺制备的具有丰富 PdFe 合金-FeC 界面的 PdFe 催化剂，在 300 ℃、5 MPa 和 6000 mL g h 下，HA 产量可达 86.5 mg·gh，选择性为 26.5%。加速失活测试表明，PdFe 催化剂在恶劣条件下比广泛研究的 CuFe 基催化剂表现出更好的耐久性。多个原位表征结果揭示了 PdFe 合金-FeC 界面上 HA 合成的协同机制，其中 PdFe 合金负责 CO 形成和非解离活化，而 FeC 相促进 CO 解离和链增长。