A tailored multi-functional catalyst for ultra-efficient styrene production under a cyclic redox scheme

Xing Zhu; Yunfei Gao; Xijun Wang; Vasudev Haribal; Junchen Liu; Luke M. Neal; Zhenghong Bao; Zili Wu; Hua Wang; Fanxing Li

doi:10.1038/s41467-021-21374-2

A tailored multi-functional catalyst for ultra-efficient styrene production under a cyclic redox scheme

Xing Zhu, Yunfei Gao, Xijun Wang, Vasudev Haribal, Junchen Liu, Luke M. Neal, Zhenghong Bao, Zili Wu, Hua Wang, Fanxing Li

Surface Chemistry & Catalysis Group

Research output: Contribution to journal › Article › peer-review

61 Scopus citations

Abstract

Styrene is an important commodity chemical that is highly energy and CO₂ intensive to produce. We report a redox oxidative dehydrogenation (redox-ODH) strategy to efficiently produce styrene. Facilitated by a multifunctional (Ca/Mn)_1−xO@KFeO₂ 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% CO₂ emission reduction. The redox catalyst is composed of a catalytically active KFeO₂ shell and a (Ca/Mn)_1−xO core for reversible lattice oxygen storage and donation. The lattice oxygen donation from (Ca/Mn)_1−xO sacrificially stabilizes Fe³⁺ 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.

Original language	English
Article number	1329
Journal	Nature Communications
Volume	12
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-21374-2
State	Published - Dec 1 2021

Funding

This work was supported by the US Department of Energy (RAPID Subaward DE-EE0007888-05-6), the US National Science Foundation (Award No. CBET-1923468), and the Kenan Institute for Engineering, Technology and Science at NC State University. Z.B. and Z.W. were supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program. Part of the work including in situ IR and Raman was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. TEM and in situ XRD were conducted in Analytical Instrumentation Facility (AIF) at North Carolina State University. LEIS was done at the operando facilities at Leigh University, under the help of Dr. Henry Luftman and Dr. Israel E. Wachs. M\u00F6ssbauer spectroscopy was done at Dalian Institute of Chemical Physics, under the help of Dr. Chuande Huang and Dr. Xiaodong Wang.

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title = "A tailored multi-functional catalyst for ultra-efficient styrene production under a cyclic redox scheme",

abstract = "Styrene is an important commodity chemical that is highly energy and CO2 intensive to produce. We report a redox oxidative dehydrogenation (redox-ODH) strategy to efficiently produce styrene. Facilitated by a multifunctional (Ca/Mn)1−xO@KFeO2 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% CO2 emission reduction. The redox catalyst is composed of a catalytically active KFeO2 shell and a (Ca/Mn)1−xO core for reversible lattice oxygen storage and donation. The lattice oxygen donation from (Ca/Mn)1−xO sacrificially stabilizes Fe3+ 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.",

author = "Xing Zhu and Yunfei Gao and Xijun Wang and Vasudev Haribal and Junchen Liu and Neal, {Luke M.} and Zhenghong Bao and Zili Wu and Hua Wang and Fanxing Li",

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AU - Liu, Junchen

AU - Neal, Luke M.

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AU - Wu, Zili

AU - Wang, Hua

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N2 - Styrene is an important commodity chemical that is highly energy and CO2 intensive to produce. We report a redox oxidative dehydrogenation (redox-ODH) strategy to efficiently produce styrene. Facilitated by a multifunctional (Ca/Mn)1−xO@KFeO2 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% CO2 emission reduction. The redox catalyst is composed of a catalytically active KFeO2 shell and a (Ca/Mn)1−xO core for reversible lattice oxygen storage and donation. The lattice oxygen donation from (Ca/Mn)1−xO sacrificially stabilizes Fe3+ 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.

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A tailored multi-functional catalyst for ultra-efficient styrene production under a cyclic redox scheme

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