Oxygen Defect-Rich WO3−x–W3N4 Mott–Schottky Heterojunctions Enabling Bidirectional Catalysis for Sulfur Cathode,Advanced Functional Materials

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Oxygen Defect-Rich WO3−x–W3N4 Mott–Schottky Heterojunctions Enabling Bidirectional Catalysis for Sulfur Cathode
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-08-30 , DOI: 10.1002/adfm.202306578
Dan Zhang ₁ , Tengfei Duan ₁ , Yixin Luo ₁ , Sisi Liu ₁ , Wanqi Zhang ₁ , Yongqian He ₁ , Kai Zhu ₁ , Li Huang ₁ , Yue Yang ₁ , Ruizhi Yu ₂ , Xiukang Yang ₁ , Hongbo Shu ₁ , Yong Pei ₁ , Xianyou Wang ₁ , Manfang Chen ₁

Affiliation

The serious shuttle effect and intrinsically sluggish oxidation–reduction reaction kinetics of polysulfides severely hinder the practical commercialization of lithium–sulfur (Li–S) batteries. Herein, oxygen-defect-rich WO₃₋_x–W₃N₄ Mott–Schottky heterojunctions are designed as efficient catalysts. Based on theoretical calculations and comprehensive experimental characterization, WO₃₋_x–W₃N₄ exhibits a lower free energy change (1.03 eV) and Li₂S decomposition energy barrier (0.92 eV) than WO₃ and W₃N₄, which significantly enhances the sulfur reduction reaction (SRR) activity. Furthermore, a relationship between the catalytic activity and the energy gaps in the d and p bands centers (Δd–p) is also established, with the low Δd–p of the heterojunction leading to a lower antibonding state energy, which promotes electron transfer and interfacial redox kinetics. Oxygen vacancies can improve the catalytic effect without affecting adsorption. Hence, the Li–S battery using WO₃₋_x–W₃N₄@CC/S exhibited outstanding rate and duration performance (913.9 mAh g^–1 at 2 C, stable 400 cycles at 1 C). Impressively, the battery achieves a high areal capacity of 5.0 mAh cm⁻² under a high sulfur loading of 4.98 mg cm⁻².

中文翻译：

富氧缺陷的WO3−x–W3N4莫特–肖特基异质结实现硫阴极的双向催化

多硫化物严重的穿梭效应和本质上缓慢的氧化还原反应动力学严重阻碍了锂硫（Li-S）电池的实际商业化。在此，富氧缺陷的WO ₃₋_x –W ₃ N ₄莫特-肖特基异质结被设计为有效的催化剂。基于理论计算和综合实验表征，WO ₃₋_x –W ₃ N ₄表现出比WO ₃和W ₃ N ₄更低的自由能变化（1.03 eV）和Li ₂ S分解能垒（0.92 eV），显着降低了Li 2 S的分解能垒。增强硫还原反应（SRR）活性。此外，还建立了催化活性与d和p带中心的能隙（Δd -p ）之间的关系，异质结的低Δd -p导致较低的反键态能量，从而促进电子转移和界面氧化还原动力学。氧空位可以提高催化效果而不影响吸附。_{因此，使用WO 3−}_x –W ₃ N ₄ @CC/S的Li–S电池表现出出色的倍率和持续时间性能（2 C下为913.9 mAh g ^–1，1 C下稳定循环400次）。^{令人印象深刻的是，该电池在4.98 mg cm -2}的高硫负载下实现了5.0 mAh cm ^-2的高面积容量。

更新日期：2023-08-30

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