Zhu Xing, Gao Yunfei, Wang Xijun, Haribal Vasudev, Liu Junchen, Neal Luke M, Bao Zhenghong, Wu Zili, Wang Hua, Li Fanxing
Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, NC, USA.
State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization, Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology, Kunming, China.
Nat Commun. 2021 Feb 26;12(1):1329. doi: 10.1038/s41467-021-21374-2.
Styrene is an important commodity chemical that is highly energy and CO intensive to produce. We report a redox oxidative dehydrogenation (redox-ODH) strategy to efficiently produce styrene. Facilitated by a multifunctional (Ca/Mn)O@KFeO core-shell redox catalyst which acts as (i) a heterogeneous catalyst, (ii) an oxygen separation agent, and (iii) a selective hydrogen combustion material, redox-ODH auto-thermally converts ethylbenzene to styrene with up to 97% single-pass conversion and >94% selectivity. This represents a 72% yield increase compared to commercial dehydrogenation on a relative basis, leading to 82% energy savings and 79% CO emission reduction. The redox catalyst is composed of a catalytically active KFeO shell and a (Ca/Mn)O core for reversible lattice oxygen storage and donation. The lattice oxygen donation from (Ca/Mn)O sacrificially stabilizes Fe in the shell to maintain high catalytic activity and coke resistance. From a practical standpoint, the redox catalyst exhibits excellent long-term performance under industrially compatible conditions.
苯乙烯是一种重要的化工商品，其生产过程能源消耗大且碳排放高。我们报道了一种氧化还原氧化脱氢（redox-ODH）策略，可高效生产苯乙烯。在多功能（Ca/Mn）O@KFeO核壳氧化还原催化剂的促进下，该催化剂兼具（i）非均相催化剂、（ii）氧分离剂和（iii）选择性氢燃烧材料的作用，redox-ODH可将乙苯自动热转化为苯乙烯，单程转化率高达97%，选择性大于94%。相对而言，这比商业脱氢法的产率提高了72%，节能82%，碳排放减少79%。该氧化还原催化剂由具有催化活性的KFeO壳层和用于可逆晶格氧储存与释放的（Ca/Mn）O核组成。（Ca/Mn）O释放的晶格氧可牺牲性地稳定壳层中的铁，以保持高催化活性和抗结焦性能。从实际应用角度看，该氧化还原催化剂在工业兼容条件下表现出优异的长期性能。
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