LANGMUIR
·
2025
·
IF 3.9
Ruoyi Chen,Fuding Tan,Xiang Wang,Yuxin Hou,Ming Ouyang,Xingyun Guan,Peng Liu,Zuliang Wu,Shuiliang Yao,Steven L. Suib,Daiqi Ye
The transportation and transformation of biogenic isoprene are vital for the organic carbon cycle in the troposphere. As a typical mineral with high oxidation potential, Fe-substituted cryptomelane oxidizes the surface monolayer of isoprene into formic and acetic acids, and simultaneously, the Mn4+ ions in the structure are reduced to Mn3+ and Mn2+. The flow of H2O in isoprene decreases the adsorption and oxidation of isoprene significantly, even at low relative humidity (10%). As physisorbed H2O retains Fe-substituted cryptomelane’s crystal structure and oxidation ability, the adsorption and oxidation capacity recovers when H2O is absent in the isoprene flow. Theoretical calculations on (001) surfaces show that isoprene prefers to be adsorbed by the Fe3+ site and H2O tends to form hydrogen bonds. Due to the decrease in total adsorption energy of H2O and isoprene, Fe-substituted cryptomelane favors the adsorption of H2O in the flow of humid isoprene. The low oxidation performance at ambient relative humidity suggests that direct oxidation by aerosols of mineral dust might not be the transformation pathway of biogenic isoprene at night.
研究领域:
大气科学
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环境化学
✓ 已验证
DOI
PubMed
高影响因子
Small
·
2021
·Vol. 18
·期 6
·2106273
·
IF 13.281
Huan Liu,Na Li,Weibin Zhang,Shiwei Zhang,Jianchuan Wang,Yong Du
Heterogeneous atoms substitution is an efficient method for promoting Li + storage of transition metal oxides. Herein, a series of Fe-substituted MnO solid solutions with different Fe contents are synthesized by a feasible solid-phase method. The synergistic effects between heterogeneous atoms and rich vacancies are synchronously obtained, which hold distinctive electronic structures and substantial active sites. When optimized Mn 0.55 Fe 0.45 O solid solution as anodes for lithium-ion batteries, pre-prepared electrodes exhibit reversible lithium storage of 1286.9 mAh g –1 at 1 A g −1 after 400 cycles and even 628.1 mAh g –1 at 2 A g –1 after 1000 cycles. The LiCoO 2 //Mn 0.55 Fe 0.45 O full cells are assembled, achieving the reversible capacity of 130.2 and 111.3 mAh g –1 after 150 cycles at 0.1 and 0.2 A g –1 , respectively. Density functional theory calculations also authenticate that the electrochemical activity can be markedly boosted by the heterogeneous atoms substituted Mn 1 -x Fe x O solid solution.
研究领域:
材料科学
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电化学
·
电池技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hailong Liao,Heping Xie,Shuo Zhai,Ling Fu,Yuan Zhang,Senran Hao,Bin Chen,Chuanxin He,Zongping Shao
Aqueous Zn-CO 2 batteries are a new technology for reducing carbon dioxide emissions and converting CO 2 into valuable products. The development of high-performance catalysts is crucial for improving the efficiency of the CO 2 reduction reaction(CO 2 RR) in these batteries. The technical challenges of CO 2 RR catalysts include high cost, complicated synthesis and low Faraday efficiency. In this study, we developed an efficient and cost-effective CO 2 RR perovskite catalyst, by partially substituting Fe to the B site of precious metal-free La 0.5 Sr 0.5 MnO 3 (LSM) perovskite. Comprehensive investigation into the Structure, morphology, coordination information and electrochemical performance of pristine La 0.5 Sr 0.5 MnO 3 (LSM) and substituted La 0.5 Sr 0.5 Fe 0.6 MnO 3 (LSF 0.6 M) catalysts were conducted, LSF 0.6 M catalyst shows enhanced electrochemical performance, Faraday efficiency, battery durability and battery power density than LSM. Specifically, the Fe-doped catalyst shows a significant improvement in CO 2 reduction reaction (CO 2 RR) performance, with an 80% increase in current density, an 82% Faraday efficiency, and a 50% increase in power density of Zn-CO 2 battery. Characterization experimental results and DFT calculation reveal that Fe substitution can increase the perovskite lattice size to favor CO 2 absorption and *COOH formation, thus the improved CO yields. These analyses provided insights into the underlying mechanisms of the catalyst's performance in CO 2 RR within the battery system. These results highlight LSF 0.6 M perovskite as a very promising CO 2 RR electrocatalyst for Zn-CO 2 battery.
研究领域:
材料科学
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能源科学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Physics
·
2021
·
IF 9.298
A. Wang,Y. Hu,H. Wang,Y. Cheng,T. Thomas,R. Ma,J. Wang
To improve the structure-dominant activity, rational design of oxide-based materials remains challengeable in bifunctional oxygen electrocatalysis , especially from the perspective of electronic modulation. Herein, we demonstrate that the electron configuration of inverse spinel NiCo 2 O 4 can be activated by controllable substitution of Fe into the octahedral centers. Fe-substituted NiCo 2 O 4 nanoparticles embedded in porous N-doped carbon nanofibers (NiCo 2- x Fe x O 4 /NCNF), which were synthesized by scalable electrospinning, exhibit a correlated relationship with Fe atomic content and achieve an optimal bifunctional activity (ΔE = 0.74 V) at 0.25 at.%. Theoretical calculation shows that the substitution of Co 3+ by Fe 3+ modulates the electrons filling in e g orbital of octahedral cation via delocalizing the electrons around O anions. The increased density of states around the Fermi level further regulate the adsorption energy of oxygen intermediates and lead to better bifunctional performance than commercial Pt/C + RuO 2 in rechargeable Zn-air battery. This work provides a new pathway to develop cost-effective bifunctional electrocatalysts for electrochemical energy storage and conversion .
研究领域:
材料科学
·
电化学
·
储能与转换
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）