Non-bonding modulations between single atomic cerium and monodispersed selenium sites towards efficient oxygen reduction
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Yaping Du1(
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Currently, dual atomic catalysts (DACs) with neighboring active sites for oxygen reduction reaction (ORR) still meet lots of challenges in the synthesis, especially the construction of atomic pairs of elements from different blocks of the periodic table. Herein, a “rare earth (Ce)-metalloid (Se)” non-bonding heteronuclear diatomic electrocatalyst has been constructed for ORR by rational coordination and carbon support defect engineering. Encouraging, the optimized Ce-Se diatomic catalysts (Ce-Se DAs/NC) displayed a half-wave potential of 0.886 V vs. reversible hydrogen electrode (RHE) and excellent stability, which surpass those of separate Ce or Se single atoms and most single/dual atomic catalysts ever reported. In addition, a primary zinc-air battery constructed using Ce-Se DAs/NC delivers a higher peak power density (209.2 mW·cm−2) and specific capacity (786.4 mAh·gZn−1) than state-of-the-art noble metal catalysts Pt/C. Theoretical calculations reveal that the Ce-Se DAs/NC has improved the electroactivity of the Ce-N4 region due to the electron transfer towards the nearby Se specific activity (SA) sites. Meanwhile, the more electron-rich Se sites promote the adsorptions of key intermediates, which results in the optimal performances of ORR on Ce-Se DAs/NC. This work provides new perspectives on electronic structure modulations via non-bonded long-range coordination micro-environment engineering in DACs for efficient electrocatalysis.
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We gratefully acknowledge the support from the National Key R&D Program of China (No. 2021YFA1501101), the National Natural Science Foundation of China (No. 21971117), the National Natural Science Foundation of China/Research Grant Council of Hong Kong Joint Research Scheme (No. N_PolyU502/21), the National Natural Science Foundation of China/Research Grants Council (RGC) of Hong Kong Collaborative Research Scheme (No. CRS_PolyU504/22), the Functional Research Funds for the Central Nankai University (No. 63186005), the Tianjin Key Lab for Rare Earth Materials and Applications (No. ZB19500202), the Open Funds (No. RERU2019001) of the State Key Laboratory of Rare Earth Resource Utilization, the 111 Project (No. B18030) from China, the Beijing-Tianjin-Hebei Collaborative Innovation Project (No. 19YFSLQY00030), the Outstanding Youth Project of Tianjin 21 Natural Science Foundation (No. 20JCJQJC00130), the Key Project of Tianjin Natural Science Foundation (No. 20JCZDJC00650), the funding for Projects of Strategic Importance of The Hong Kong Polytechnic University (Project Code: 1-ZE2V), the Shenzhen Fundamental Research Scheme-General Program (No. JCYJ20220531090807017), the Natural Science Foundation of Guangdong Province (No. 2023A1515012219), and the Departmental General Research Fund (Project Code: ZVUL) from The Hong Kong Polytechnic University. B. L. H. also thanks the support from Research Centre for Carbon-Strategic Catalysis (RC-CSC), Research Institute for Smart Energy (RISE), and Research Institute for Intelligent Wearable Systems (RI-IWEAR) of the Hong Kong Polytechnic University.
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