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Abstract In situ construction of active structure under reaction conditions is highly desired but still remains challenging in many important catalytic processes. Herein, we observe structural evolution of molybdenum oxide (MoO x ) into highly active molybdenum carbide (MoC x ) during reverse water‐gas shift (RWGS) reaction. Surface oxygen atoms in various Mo‐based catalysts are removed in H 2 ‐containing atmospheres and then carbon atoms can accumulate on surface to form MoC x phase with the RWGS reaction going on, both of which are enhanced by the presence of intercalated H species or Pt‐dopants in MoO x . The structural evolution from MoO x to MoC x is accompanied by enhanced CO 2 conversion, which is positively correlated with the surface C/Mo ratio but negatively with the surface O/Mo ratio. As a result, an unprecedented CO formation rate of 7544.6 mmol ⋅ g catal −1 ⋅ h −1 at 600 °C has been achieved over in situ carbonized H‐intercalated MoO 3 catalyst, which is even higher than those from noble metal catalysts. During 100 h stability test only a minimal deactivation rate of 2.3 % is observed.
Du et al. (Thu,) studied this question.