Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO <sub>2</sub> hydrogenation-Reference-Cited by-同舟云学术

Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO ₂ hydrogenation

Published:2022-02-04 Issue:5 Volume:8 Page:
ISSN:2375-2548
Container-title:Science Advances
language:en
Short-container-title:Sci. Adv.

Author:

Zhu Jie¹^ORCID,Wang Peng²,Zhang Xiaoben³^ORCID,Zhang Guanghui¹^ORCID,Li Rongtan⁴^ORCID,Li Wenhui¹^ORCID,Senftle Thomas P.²^ORCID,Liu Wei³^ORCID,Wang Jianyang¹,Wang Yanli¹,Zhang Anfeng¹,Fu Qiang³⁴^ORCID,Song Chunshan¹⁵^ORCID,Guo Xinwen¹^ORCID

Affiliation:

1. State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China.

2. Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX 77005, USA.

3. Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.

4. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.

5. Department of Chemistry, Faculty of Science, The Chinese University of Hong Kong, Shatin, NT, Hong Kong, China.

Abstract

Identifying the dynamic structure of heterogeneous catalysts is crucial for the rational design of new ones. In this contribution, the structural evolution of Fe(0) catalysts during CO 2 hydrogenation to hydrocarbons has been investigated by using several (quasi) in situ techniques. Upon initial reduction, Fe species are carburized to Fe 3 C and then to Fe 5 C 2 . The by-product of CO 2 hydrogenation, H 2 O, oxidizes the iron carbide to Fe 3 O 4 . The formation of Fe 3 O 4 @(Fe 5 C 2 +Fe 3 O 4 ) core-shell structure was observed at steady state, and the surface composition depends on the balance of oxidation and carburization, where water plays a key role in the oxidation. The performance of CO 2 hydrogenation was also correlated with the dynamic surface structure. Theoretical calculations and controll experiments reveal the interdependence between the phase transition and reactive environment. We also suggest a practical way to tune the competitive reactions to maintain an Fe 5 C 2 -rich surface for a desired C 2+ productivity.

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

Reference62 articles.

1. Reversible loss of core–shell structure for Ni–Au bimetallic nanoparticles during CO2 hydrogenation

2. Structural Evolution and Dynamics of an In2O3 Catalyst for CO2 Hydrogenation to Methanol: An Operando XAS-XRD and In Situ TEM Study

3. Variation in the In2O3 Crystal Phase Alters Catalytic Performance toward the Reverse Water Gas Shift Reaction

4. Reaction-driven surface reconstruction of ZnAl2O4 boosts the methanol selectivity in CO2 catalytic hydrogenation

5. Molybdenum Carbide as Alternative Catalysts to Precious Metals for Highly Selective Reduction of CO2to CO

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