Asymmetric Co?N3P1 Trifunctional Catalyst with Tailored Electronic Structures Enabling Boosted Activities and Corrosion Resistance in an Uninterrupted Seawater Splitting System,Advanced Materials

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Asymmetric Co?N3P1 Trifunctional Catalyst with Tailored Electronic Structures Enabling Boosted Activities and Corrosion Resistance in an Uninterrupted Seawater Splitting System
Advanced Materials ( IF 27.4 ) Pub Date : 2022-07-04 , DOI: 10.1002/adma.202204021
Xingkun Wang ₁ , Xinkun Zhou ₂ , Cheng Li _{3,

4} , Hanxu Yao _{1,

2} , Canhui Zhang ₁ , Jian Zhou ₁ , Ren Xu ₁ , Lei Chu ₁ , Huanlei Wang ₁ , Meng Gu ₃ , Heqing Jiang ₂ , Minghua Huang ₁

Affiliation

Employing seawater splitting systems to generate hydrogen can be economically advantageous but still remains challenging, particularly for designing efficient and high Cl⁻-corrosion resistant trifunctional catalysts toward the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). Herein, single CoNC catalysts with well-defined symmetric CoN₄ sites are selected as atomic platforms for electronic structure tailoring. Density function theory reveals that P-doping into CoNC can lead to the formation of asymmetric CoN₃P₁ sites with symmetry-breaking electronic structures, enabling the affinity of strong oxygen-containing intermediates, moderate H adsorption, and weak Cl⁻ adsorption. Thus, ORR/OER/HER activities and stability are optimized simultaneously with high Cl⁻-corrosion resistance. The asymmetric CoN₃P₁ structure based catalyst with boosted ORR/OER/HER performance endows seawater-based Zn–air batteries (S-ZABs) with superior long-term stability over 750 h and allows seawater splitting to operate continuously for 1000 h. A self-driven seawater splitting powered by S-ZABs gives ultrahigh H₂ production rates of 497 μmol h⁻¹. This work is the first to advance the scientific understanding of the competitive adsorption mechanism between Cl⁻ and reaction intermediates from the perspective of electronic structure, paving the way for synthesis of efficient trifunctional catalysts with high Cl⁻-corrosion resistance.

中文翻译：

具有定制电子结构的不对称 Co?N3P1 三功能催化剂可在不间断的海水分解系统中提高活性和耐腐蚀性

使用海水分解系统产生氢气在经济上具有优势，但仍然具有挑战性，特别是对于设计用于氧还原反应 (ORR)、析氧反应 (OER) 和析氢反应的高效和高耐Cl ^-腐蚀的三功能催化剂。她）。在此，选择具有明确对称CoN 4 位点的单一CoNC催化剂作为电子_结构调整的原子平台。密度函数理论表明，P掺杂CoNC可以导致不对称CoN 3 _P1_的形成具有对称破坏电子结构的位点，能够实现强含氧中间体的亲和力、适度的 H 吸附和弱的 Cl ^-吸附。因此，ORR/OER/HER 活性和稳定性与高 Cl ^-耐腐蚀性同时得到优化。具有增强的 ORR/OER/HER 性能的不对称Co N ₃ P ₁结构基催化剂赋予海水基锌空气电池（S-ZABs）超过 750 小时的出色长期稳定性，并允许海水分解连续运行 1000 H。由 S-ZAB 驱动的自驱动海水分解产生 497 μmol h ^{-1的超高 H}₂产率. 该工作首次从电子结构的角度推进了对Cl ^{-与反应中间体之间竞争吸附机制的科学认识，为合成具有高Cl}^-耐腐蚀性的高效三功能催化剂铺平了道路。

更新日期：2022-07-04

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