Interfacial Robustness and Improved Kinetics of Single-Crystal Ni-Rich Co-Free Cathodes Enabled by Surface Crystal-Facet Modulation.

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-09-18 Epub Date: 2024-09-03 DOI:10.1021/acs.nanolett.4c01816

Zhiming Xiao, Xinyou He, Fangyong Yu, Bao Zhang, Xing Ou

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引用次数: 0

Abstract

The elimination of Co from Ni-rich layered cathodes is critical to reduce the production cost and increase the energy density for sustainable development. Herein, a delicate strategy of crystal-facet modulation is designed and explored, which is achieved by simultaneous Al/W-doping into the precursors, while the surface role of the crystal-facet is intensively revealed. Unlike traditional studies on crystal structure growth along a certain direction, this work modulates the crystal-facet at the nanoscale based on the effect of W-doping dynamic migration with surface energy, successfully constructing the core-shell (003)/(104) facet surface. Compared to the (003) plane, the induced (104) facet at the surface can provide more space for Li⁺-activity, enabling lower interfacial polarization and higher Li⁺-transport rate. Additionally, bulk Al-doping is beneficial for enhancing the Li⁺-diffusion from the exterior surface to the interior lattice. With improved interfacial stability and restrained surface erosion, the product exhibits superior capacity retention and boosted rate performance under the elevated temperature.

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通过表面晶面调制实现单晶富镍无共价阴极的界面稳健性和动力学改进

从富镍层状阴极中去除钴对于降低生产成本和提高能量密度以实现可持续发展至关重要。本文设计并探索了一种微妙的晶体面调制策略，通过在前驱体中同时掺入 Al/W 来实现，同时深入揭示了晶体面的表面作用。与传统的晶体结构沿某一方向生长的研究不同，该研究基于 W 掺杂动态迁移对表面能的影响，在纳米尺度上对晶体面进行调制，成功构建了核壳（003）/（104）面表面。与（003）面相比，表面的诱导（104）面可为 Li+ 活性提供更大的空间，从而实现更低的界面极化和更高的 Li+ 传输速率。此外，大量掺铝有利于增强 Li+ 从外表面向内部晶格的扩散。随着界面稳定性的提高和表面侵蚀的抑制，该产品在高温条件下表现出卓越的容量保持能力和更高的速率性能。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.