CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yan Liu,Ling Zhang,Kaiyang Guo,Jingyuan Zhao,Yonglei Xing,Zhuosen Wang,Yapeng Tian,Xinwei Cui
Intercalation pseudocapacitance is the key point to achieving the balance between the volumetric capacitance and the rate performance of energy storage. However, the low pseudocapacitive reactivity of the active center still limits the energy density of the pseudocapacitance devices. Herein, we propose a strategy that regulates the p - d hybridization of confined MXene via the co-doping of B and O atoms (BO-MXene) for outstanding electrochemical performance. Both experiments and density functional theory (DFT) reveal that the inner doped O atoms in low 2 p orbital energy strengthen the hybridization of Ti and electron-deficient B in MXene for high retention of B atoms, weaken the Ti-O covalency in MXene. As a result, the weakened p - d hybridization of Ti and O for the outer surface and strengthened p - d hybridization of Ti and B for the inner, promote the adsorption of protons and electron transfer, respectively. Further, the BO-MXene-based hybrid supercapacitors achieve a significant volumetric energy density of 56.86 Wh L -1 at 25.6 kW L -1 . This electronic structure via tuning the p - d hybridization in MXene proposes a new path for designing proton-confined intercalation pseudocapacitance.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xianwei Li,Shuangxiu Ma,Fang Luo,Zehui Yang
Electrochemical hydrogenerations of nitrogen and oxygen molecules are of significance for nitrogen reduction and oxygen reduction reactions. Strengthening the binding between active sites and gaseous molecules is beneficial for enhancing the catalytic performance, especially in NRR catalysis. In this work, we have engineered the oxygen vacancies in Co 3 O 4 nanoparticles to boost the catalytic activity towards NRR and ORR. Ascribing to the p-d hybridization between Co and N atoms, N 2 electrochemical adsorption is promoted and the related energy barrier of N 2 protonation is significantly decreased by 50%; as a consequence, Faradaic efficiency is 11.2% at −0.4 V vs. RHE, 3-fold higher than Co 3 O 4 /CNT; moreover, due to the oxygen vacancies in Co 3 O 4-x /CNT leading to a higher oxophilicity, Co 3 O 4-x /CNT showed a better selectivity in ORR catalysis and kinetic current density at 0.85 V vs. RHE is boosted by 2.4 times. Consequently, Co 3 O 4-x /CNT exhibits a better rechargeable zinc air battery performance than Pt/C-IrO 2 by a factor of 2.2.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Yutong Tong,Butian Chen,Chong Liu,Ruoyu Wang,Dewen Wang,Tianran Zhang,Xiaobai Ma,Limei Sun,Jinbo Yang,Wenyun Yang,Xiangfeng Liu
Halide solid electrolytes (SEs) show great potential in all-solid-state batteries (ASSBs) because of their high ionic conductivity and high oxidative stability. But the long-term cycling stability remains a major concern due to the cathode/halide interface side reactions, especially under high current density. Herein, a s-p-d orbital hybridization strategy is proposed via introducing Zr 4+ and F − into Li 3 InCl 6 (LIC-ZrF 4 ) to regulate the electron localization structure around the central In 3+ . The electron transfer between the cation and Cl is alleviated by the enlarged bandgap (4.485–4.894 eV) with ZrF 4 introduction, and more electrons aggregate around In 3+ after s-p-d hybridization among Zr, In, and Cl. This effectively prevents LIC-ZrF 4 from being attacked by O atoms in LiNi 0 . 8 Co 0 . 1 Mn 0 . 1 (NCM811) and significantly suppresses the interface side reactions. The in situ formed LiF-containing layer further enhances the interface stability. The assembled ASSB (NCM811/LIC-ZrF 4 /LPSC/Li-In) exhibits a state-of-the-art capacity retention (96.7%@500cycles@1C; 80.7%@1600 cycles@2C). Furthermore, the ionic conductivity of LIC-ZrF 4 is also enhanced from 0.6 to 1.5 mS cm −1 while the electronic conductivity is decreased from 3.66 × 10 −8 to 8.39 × 10 −9 S cm −1 . This work highlights the crucial role of s-p-d hybridization on the electron localization regulation and the interface stability, and presents some distinct insights into developing high-performance halides-based ASSBs.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2023
·Vol. 15
·期 8
·3772-3779
·
IF 6.7
Qiaoli Chen,Hui Jin,Tianchun Cheng,Zhi Wang,Yaoyao Ren,Jinshu Tian,Yihan Zhu
Proton-exchange membrane fuel cells are considered as promising energy-conversion devices. Alloying 3d transition metals with noble metals not only highly improves the performance of noble metal-based catalysts towards electrocatalytic reactions in fuel cells due to d–d hybridization interaction but also decreases the total cost. However, the rapid leaching of transition metal atoms leads to a fast decay of the activity, which seriously affects the performance of the fuel cell. Herein, alloyed Pd-main group metal (e.g. Pb, Bi, Sn) ultrathin nanowires were realized by a facile one-step wet-chemical strategy. The content of the main group metal could be tuned in a certain range while maintaining the same one-dimensional ultrathin nanowire morphology, which provided a large surface area and many more active sites. These Pd-based alloys showed a significant improvement in electrocatalytic activity and durability towards the oxygen reaction reaction as well as ethanol oxidation reaction. Optimal activity occurred when a small amount of main group metal existed, which could be explained through calculations by a strong p–d hybridization interaction between the main group metal and Pd to optimize the surface electronic structure collaboratively. Besides, high stability was achieved, which could be ascribed to the increased antioxidant activity of Pd by the main group metal. Furthermore, the low amount of the main group metal atoms also prevented them from leaching out of the crystal lattice.
研究领域:
材料科学
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纳米技术
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电化学
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能量转换设备
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Guanhua Zhang,Mingwang Lu,Qitong Sheng,Guangjian Xing,Xiaojing Yang,Xiaofei Yu,Xinghua Zhang,Zunming Lu,Lanlan Li
The development of highly efficient and stable bifunctional electrocatalysts capable of simultaneously catalyzing the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is critical for advancing zinc-air batteries (ZABs). However, the linear scaling relationship (LSR) governing the adsorption energies of oxygen species imposes constraints on the concurrent enhancement of ORR and OER performance. In this study, we report the synthesis of a novel FeSn/NC catalyst that exhibits strong p-d orbital hybridization by incorporating p-block Sn metal into d-block Fe metal. This strategy facilitates the manipulation of the d-band center and enables the effective formation of low-spin (LS) Fe 3+ simultaneously. The regulation of the d-band center is identified as an effective strategy to enhance the adsorption energy of OOH* and OH* intermediates, while the LS Fe 3+ configuration can effectively weaken the adsorption strength of the O* intermediate. Consequently, this p-d hybridized Fe-based catalyst successfully overcomes the constraints imposed by LSR, thereby boosting bifunctional activity for both ORR and OER. The synthesized FeSn/NC catalyst demonstrates exceptional bifunctional performance with a potential difference (ΔE) of 0.65 V between ORR and OER activities. Furthermore, ZAB based on FeSn/NC achieves an impressive peak power density of 186.0 mW cm −2 , while maintaining stable operation over 700 h during cycling tests. This work offers new insights into designing high-performance bifunctional electrocatalysts through strategies involving synergistic modulation of d-band center and spin state.
研究领域:
电化学
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材料科学
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催化
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能量存储与转换
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）