Nano-Micro Letters
·
2023
·Vol. 16
·期 1
·1-18
·
IF 26.6
Li Xudong,Qiang Zhuomin,Han Guokang,Guan Shuyun,Zhao Yang,Lou Shuaifeng,Zhu Yongming
High-entropy catalysts featuring exceptional properties are, in no doubt, playing an increasingly significant role in aprotic lithium-oxygen batteries. Despite extensive effort devoted to tracing the origin of their unparalleled performance, the relationships between multiple active sites and reaction intermediates are still obscure. Here, enlightened by theoretical screening, we tailor a high-entropy perovskite fluoride (KCoMnNiMgZnF 3 -HEC) with various active sites to overcome the limitations of conventional catalysts in redox process. The entropy effect modulates the d -band center and d orbital occupancy of active centers, which optimizes the d – p hybridization between catalytic sites and key intermediates, enabling a moderate adsorption of LiO 2 and thus reinforcing the reaction kinetics. As a result, the Li–O 2 battery with KCoMnNiMgZnF 3 -HEC catalyst delivers a minimal discharge/charge polarization and long-term cycle stability, preceding majority of traditional catalysts reported. These encouraging results provide inspiring insights into the electron manipulation and d orbital structure optimization for advanced electrocatalyst.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Yongqi Zhao,Junjie Jiang,Yang Zou,Pu Wang,Xue Li,Xiaolong Liu,Tingyu Zhu
The catalyst cost is a key factor limiting the CO purification of sintering flue gas. Here, an ultra-low-loading high-entropy catalyst was prepared by simple calcination process. By anchoring multiple active metal sites in the stable anatase TiO 2 phase, it shows efficient CO catalytic oxidation activity. The metal components (Pt, Mn, Fe, Co, Ni) were uniformly dispersed on the surface of TiO 2 in the form of high-entropy compounds and undergo strong metal and support interaction with TiO 2 . The results showed that 0.1(PtMnFeCoNi)/TiO 2 achieved complete oxidation of CO at 230 °C, and its catalytic oxidation ability was significantly better than that of the corresponding monometallic and bimetallic catalysts. The high-entropy component adjusts the electronic environment between the TiO 2 support and the metal to promote the reduction of the Ti 3 d band gap, enhances the electron-induced ability of the catalytic system to gas molecules (CO and O 2 ), and exhibits excellent resistance to SO 2 and H 2 O. The work is of great significance to understand the synergistic regulation of catalyst activity by multiple metal at the atomic level and provides a strategy for effectively reducing the content of precious metals in the catalyst.
研究领域:
催化
·
材料科学
·
环境化学
·
纳米技术
·
表面科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2024
·Vol. 14
·期 4
·999-1007
·
IF 4.4
Ziling Liu,Jipeng Wang,Xiaoqian Gao,Yadong Bi,Chen Guo,Xinli Tong
Selective catalytic reduction of α,β-unsaturated aldehydes plays a significant role in the present chemical industry. In this article, a series of high entropy catalysts were prepared and employed to catalyze the hydrogen transfer reaction of furan-2-acrolein in alcoholic solvents. As a result, the catalyst containing inexpensive Cu, Co, Al, Ni, and Fe elements exhibited outstanding performance, in which more than 99.9% conversion and 93.3% selectivity to 2-furan propanol are obtained in the presence of the CuCoAlNiFeOx catalyst; meanwhile, the furan ring-hydrogenated products 3-(tetrahydrofuran-2-yl)propanal and 3-(tetrahydrofuran-2-yl)propan-1-ol are mainly generated using CuCoAlNiFe-250R as the catalyst. Based on the results of control experiments and catalyst characterization, it is concluded that the synergistic effect between the five different metal elements is very crucial to the prominent catalytic activity. Moreover, the presence of metal Cu is advantageous for the hydrogenation of the side chain CC and CO bonds, while the reduced state Ni is responsible for the hydrogen transfer reduction of the furan ring. This study provides an economical and facile approach for the selective reduction of aromatic α,β-unsaturated aldehydes and biomass-derived furanic derivatives.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·Vol. 30
·期 39
·e202400756
·
IF 3.9
Siyang Jin,Yu Fu,Kecheng Jie,Huan Dai,Yun Jie Luo,Liang Ye,Chaohui Zhou,Wei Xu
Graphical A high-entropy lanthanide–organic framework (HE-LnMOF) heterogeneous catalyst toward sustainable CO 2 conversion reactions. The five rare earth metals were well-dispersed and randomly distributed in the structure. The HE-LnMOF possess multiple unsaturated metal centers, abundant Lewis acid and base interaction sites at the same time. The synergistic effect of multi-metallic Ln 3+ ions endow it with outstanding catalytic performance. Multimetallic synergistic effects have the potential to improve CO 2 cycloesterification and Knoevenagel reaction processes, outperforming monometallic MOFs. The results demonstrate superior performance in these processes. To investigate this, we created and characterized a selection of single-component Ln(III)-MOFs (Ln=Eu, Tb, Gd, Dy, Ho) and high-entropy lanthanide-organic framework (HE-LnMOF) using solvent-thermal conditions. The experiments revealed that HE-LnMOF exhibited heightened catalytic efficiency in CO 2 cycloesterification and Knoevenagel reactions compared to single-component Ln(III) MOFs. Moreover, the HE-LnMOF displayed significant stability, maintaining their structural integrity after five cycles while sustaining elevated conversion and selectivity rates. The feasible mechanisms of catalytic reactions were also discussed. HE-LnMOF possess multiple unsaturated metal centers, acting as Lewis acid sites, with oxygen atoms connecting the metal, and hydroxyl groups on the ligand serving as base sites. This study introduces a novel method for synthesizing HE-LnMOF and presents a fresh application of HE-LnMOF for converting CO 2 .
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Xiaolong Wang,Juping Liu,Haiping Yang,Changzhi Li,Yang Yang
The hydrodeoxygenation (HDO) of biomass derived oils offers a viable route to produce sustainable aviation fuels, yet its large-scale application remains constrained by the reliance on noble metal catalysts. Herein, we report a high-entropy NiFeCoMo catalyst composed entirely of earth-abundant elements, which achieves noble-metal-level performance in the HDO of lignin-derived compounds. The catalyst exhibits remarkable activity and selectivity across a range of model compounds and their mixtures, reaching up to 99.9% conversion and 98.1% selectivity for methylcyclohexane even under mixed-feedstock conditions. Recyclability tests confirm excellent durability over five consecutive cycles without measurable loss of activity. Density functional theory calculations reveal that the synergistic electronic interaction among multiple metal sites induce strong hydrogen spillover, promoting the formation of oxygen vacancies that facilitate complete C-O bond cleavage. This work establishes high-entropy catalysts as a robust and sustainable alternative to precious metals for efficient biomass upgrading, offering new insights into the design of multifunctional active sites for selective hydrodeoxygenation.
研究领域:
催化
·
可再生能源
·
生物质转化
·
材料科学
·
可持续化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）