Beijing State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing China
Xin Tu
Department of Electrical Engineering and Electronics University of Liverpool Liverpool UK
Zhiwei Hu
Max Planck Institute for Chemical Physics of Solids Dresden Germany
Yinlong Zhu
Institute for Frontier Science Nanjing University of Aeronautics and Astronautics Nanjing China
Hongquan Guo
College of Energy Xiamen University Xiamen China
Zhishan Li
College of Energy Xiamen University Xiamen China
Li Zhang
College of Energy Xiamen University Xiamen China
Meilan Peng
College of Energy Xiamen University Xiamen China
Lichao Jia
School of Materials Science and Engineering, State Key Lab of Material Processing and Die & Mould Technology Huazhong University of Science and Technology Wuhan China
Meiting Yang
State Key Laboratory of Materials‐Oriented Chemical Engineering, College of Chemical Engineering Nanjing Tech University Nanjing China
Guangming Yang
State Key Laboratory of Materials‐Oriented Chemical Engineering, College of Chemical Engineering Nanjing Tech University Nanjing China
Xurong Qiao
State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University Xi'an China
Jiahui Sun
State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University Xi'an China
Xiaolu Liang
State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University Xi'an China
Zhen Zhang
State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University Xi'an China
Yanru Zhu
Beijing State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing China
Lei Shi
School of Chemical Engineering Dalian University of Technology Dalian China
Chenxing Jiang
College of Energy Xiamen University Xiamen China
Yingru Zhao
College of Energy Xiamen University Xiamen China
Jianhui Li
National Engineering Laboratory for Green Chemical Productions of Alcohols‐Ethers‐Esters, College of Chemistry and Chemical Engineering Xiamen University Xiamen China
Zongping Shao
State Key Laboratory of Materials‐Oriented Chemical Engineering, College of Chemical Engineering Nanjing Tech University Nanjing China
Xin Zhang
Beijing State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing China
Yifei Sun
Beijing State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing China
Abstract The active and stable palladium (Pd) based catalysts for CH4 conversion are of great environmental and industrial significance. Herein, we employed N2 as an optimal activation agent to develop a Pd nanocluster exsolved Ce‐incorporated perovskite ferrite catalyst toward lean methane oxidation. Replacing the traditional initiator of H2, the N2 was found as an effective driving force to selectively touch off the surface exsolution of Pd nanocluster from perovskite framework without deteriorating the overall material robustness. The catalyst showed an outstanding T50 (temperature of 50% conversion) plummeting down to 350°C, outperforming the pristine and H2‐activated counterparts. Further, the combined theoretical and experimental results also deciphered the crucial role that the atomically dispersed Ce ions played in both construction of active sites and CH4 conversion. The isolated Ce located at the A‐site of perovskite framework facilitated the thermodynamic and kinetics of the Pd exsolution process, lowering its formation temperature and promoting its quantity. Moreover, the incorporation of Ce lowered the energy barrier for cleavage of C─H bond, and was dedicated to the preservation of highly reactive PdOx moieties during stability measurement. This work successfully ventures uncharted territory of in situ exsolution to provide a new design thinking for a highly performed catalytic interface.
