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The use of p-block metals to accelerate the sulfur reduction reaction (SRR) in lithium-sulfur (Li-S) batteries is emerging. However, the d-electrons inertia of p-block metal endows the weak adsorption and catalytic ability for SRR, limiting catalyst design. Herein, we fabricate an asymmetrically coordinated p-block indium trisulfide by coordination engineering with P doping and sulfur vacancies (P-In2S3-x) for SRR. The unique coordination engineering induces the rearrangement of electrons in the s/p/d hybrid orbital, causing that P-In2S3-x shifts electron states from low to high spin, generating more unpaired electrons. The obtained high-spin configuration achieves that electron transition to a higher energy level to activate d-electrons of p-block metals, which enables a novel dp coupling between d orbitals of In atoms and the p orbitals of S atoms in LiPSs, improving adsorption and catalytic ability of p-block metals for SRR. Consequently, cell with P-In2S3-x achieves excellent capacity retention, with a very low decay rate (0.036 % per cycle at 5 C over 1000 cycles) and high performance at 0 degrees C (760 mAh g- 1 at 1 C). This study offers a strategy for modulation d-electrons activity p-block metals by tailoring electron spin to boost catalytic efficiency in Li-S batteries.
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NANO ENERGY
ISSN: 2211-2855
Year: 2025
Volume: 139
1 6 . 8 0 0
JCR@2023
CAS Journal Grade:1
Cited Count:
SCOPUS Cited Count:
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 3
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