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Promotion effect with dispersed Fe-Ni-S catalyst to facilitate hydrogenolysis of lignite and heavy residue

机译：Fe-Ni-S分散催化剂的促进作用，促进褐煤和重残渣的氢解

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摘要

Nickel sulfide is regarded as one of the most promising substitutes for the best-performing disposable molybdenum catalyst in the hydrogenolysis of lignite and heavy residue, but its practical application is hindered severely by insufficient catalytic activity and a prohibitively large dosage. Herein, we report that the issues of activity and cost of nickel sulfide can be addressed simultaneously by employing a combination of iron incorporation and a dispersing strategy via oil-soluble ligands. Motivated by first-principles calculations where iron incorporation in nickel sulfide would lead to a better activity towards the rate-limiting step of hydrogenolysis compared with nickel sulfide alone, we successfully prepared a well-dispersed Fe-Ni-S catalyst by coordinating active metal salts with carboxylate ligands and a subsequent essential sulfurization. The synthesized Fe-Ni-S catalyst outperformed not only the monometallic nickel catalyst but also the commercial molybdenum catalyst in the hydrogenolysis of lignite and heavy residue, and exhibited a high conversion efficiency, hydrogen consumption, hydrogen/carbon product atomic ratio, and dispersibility of solid residues, with an economic nickel dosage of as low as similar to 250 mu g.g(-1) Structural changes of raw coal and solid residues further confirmed the role of the Fe-Ni-S catalyst in facilitating the hydrogenolysis of lignite and heavy residue.
机译：在褐煤和重残渣的氢解中，硫化镍被认为是性能最好的一次性钼催化剂的最有希望的替代品之一，但由于催化活性不足和用量过大而严重阻碍了其实际应用。在本文中，我们报道可以通过结合使用铁结合和通过油溶性配体的分散策略同时解决硫化镍的活性和成本问题。出于第一性原理的考虑，与单独使用硫化镍相比，在硫化镍中掺入铁会导致更好的氢解限速步骤活性，我们通过配位活性金属盐成功制备了分散良好的Fe-Ni-S催化剂与羧酸盐配体和随后的基本硫化。合成的Fe-Ni-S催化剂在褐煤和重残渣的氢解中不仅表现出了单金属镍催化剂的优异性能，而且还超越了市售的钼催化剂，并且具有较高的转化效率，氢消耗量，氢碳产物原子比和高分散性。固体残渣，经济镍用量低至250 mu gg（-1），原煤和固体残渣的结构变化进一步证实了Fe-Ni-S催化剂在促进褐煤和重残渣氢解中的作用。

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