Reshaping the coordination and electronic structure of single atom sites on the right branch of ORR volcano plot

doi:10.1016/S1872-2067(23)64460-2

Chinese Journal of Catalysis ›› 2023, Vol. 50: 352-360.DOI: 10.1016/S1872-2067(23)64460-2

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Reshaping the coordination and electronic structure of single atom sites on the right branch of ORR volcano plot

Liyuan Gong^a^,^b^,^c^,¹, Ying Wang^d^,¹, Jie Liu^a^,^b^,^c^,¹, Xian Wang^a^,^b^,^c, Yang Li^a^,^b^,^c, Shuai Hou^a^,^c, Zhijian Wu^d, Zhao Jin^a^,^c^,^*(), Changpeng Liu^a^,^b^,^c, Wei Xing^a^,^b^,^c^,^*(), Junjie Ge^a^,^b^,^e^,^*()

^aState Key Laboratory of Electroanalytical Chemistry, Jilin Province Key Laboratory of Low Carbon Chemical Power Sources, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China
^bUniversity of Science and Technology of China, Hefei 230026, Anhui, China
^cLaboratory of Advanced Power Sources, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China
^dState Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China
^eDalian National Laboratory for Clean Energy, Dalian 116023, Liaoning, China

Received:2023-04-05 Accepted:2023-05-08 Online:2023-07-18 Published:2023-07-25
Contact: *E-mail: zjin@ciac.ac.cn (Z. Jin), xingwei@ciac.ac.cn (W. Xing), gejunjie@ustc.edu.cn (J. Ge).
About author:
¹ Contributed to this work equally.
Supported by:
National Key R&D Program of China(2022YFB4004100);National Natural Science Foundation of China(21875243);National Natural Science Foundation of China(21733004);Science and Technology Service Network Initiative of CAS(KFJ-STS-ZDTP-088);Jilin Province Science and Technology Development Program(20190201270JC);Jilin Province Science and Technology Development Program(20190201300JC);Jilin Province Science and Technology Development Program(20200201001JC);Special Funds for Guiding Local Scientific and Technological Development by the Central Government(2020JH6/10500021);Dalian National Laboratory for Clean Energy (DNL), CAS, the Research Innovation Fund(DNL202010)

Abstract

Abstract:

The coordination environment of atomic metal sites in single atom catalysts is of vital significance in tailoring the d-orbital states and thus the catalytic behavior towards oxygen reduction reaction (ORR), thereby offering great promise to boost activity via regulating the local chelation structure. Herein we designed a carbon coordination environment for the atomic M sites reside on the right leg of the volcano plot, to effectively counter balance the low adsorption energy of the metal center to oxygen species. Combining time-of-flight secondary ion mass spectrometry and density functional theory calculations, we unveiled the M-C coordination structure and the thus induced changes in electronic structure and ORR catalytic behavior. The reshape in coordination structure, i.e., the replacement of typical nitrogen coordination by low electronegativity carbon coordination, gives rise to exceptional intrinsic activity towards ORR. This work brings a new perspective to boost the activity of single atom catalysts on the weak bonding leg, with exceptional ORR activity being further expected through advancing the chelation structure.

Key words: Oxygen reduction reaction, Single atom catalyst, Coordination environment, Electronic structure, Adsorption energy of reaction intermediate

Liyuan Gong, Ying Wang, Jie Liu, Xian Wang, Yang Li, Shuai Hou, Zhijian Wu, Zhao Jin, Changpeng Liu, Wei Xing, Junjie Ge. Reshaping the coordination and electronic structure of single atom sites on the right branch of ORR volcano plot[J]. Chinese Journal of Catalysis, 2023, 50: 352-360.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64460-2

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Figures/Tables 5

Fig. 1. (a) Synthetic scheme for the preparation of M-C and M-N-C samples; the HAADF-STEM image of Ir-N-C (b), Ir-C (c), Pd-N-C (d), Pd-C (e), Pt-N-C (f), and Pt-C (g).

Fig. 2. EXAFS and XANES spectra of Ir-N-C (a,b), Pd-N-C (c,d), Pt-N-C (e,f), Ir-C (g,h), Pd-C (i,j) and Pt-C (k,l) and reference samples.

Fig. 3. Characteristic fragment of varied catalysts detected by ToF-SIMS. IrN4 (a), IrC4 (b), PdN2 (c) of M-N-C catalysts, and PdC4 (d), PtN4 (e), PtC4 (f) of M-C catalysts.

Fig. 4. (a) The LSV curves of Ir SACs. (b) Comparison of E1/2 of Ir based catalysts. (c) The LSV curves of Pd SACs catalysts. (d) Comparison of the Eonset of Pd SACs. (e) The LSV curves of Pt SACs. (f) Comparison of the Eonset of Pt SACs. RDE and RRDE measurements were conducted by CV in 0.1 -1.1 V at a scan rate of 10 mV s-1 at 1600 r min-1 in O2 saturated 0.1 mol L-1 HClO4.

Fig. 5. (a-c) Gibbs free energy diagrams on various sites. (d-f) ORR theoretical onset potential (fitting) versus ΔGOH* on various sites. (g-i) ΔGOH* and ORR theoretical onset potential (exact) versus Bader charge for various sites. The blue symbols are corresponding to ΔGOH* and the red symbols correspond to theoretical onset potential. The circular symbols represent the MCX site and the star symbols represent the MNX site. The insert picture is charge density difference, cyan and yellow areas represent charge density increase and decrease, respectively.

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Reshaping the coordination and electronic structure of single atom sites on the right branch of ORR volcano plot

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