ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Tingshuai Yang,Chaozhu Shu,Ruixin Zheng,Minglu Li,Zhiqian Hou,Peng Hei,Qiang Zhang,Dexin Mei,Jianping Long
Gel polymer electrolytes (GPEs) have received extensive attention due to their excellent nonflammability, leak prevention, and low cost. However, low ionic conductivity at room temperature and poor interfacial stability hinder the further application of GPEs. Here, a novel GPE based on PVDF-HFP/PMMA/SiO2 (PPSE-X, X represents the mass percentage of SiO2 in the GPE) is designed and fabricated. The synthesized PPSE-15 demonstrates an organic–inorganic double complexation structure, in which two kinds of polymer cross-link, leading to the increase of lithium-ion migration amount (tli+) in PPSE-15. Moreover, polar functional group (Si–O) in the nanometer SiO2 promotes the lithium salt dissociation, regulates the Li+ deposition and thus inhibits the production of lithium dendrite. The Li/PPSE-15/Li symmetric cell can run steadily for more than 750 h at a current density of 0.5 mA cm–2. Not only that, the Li–O2 battery assembled with PPSE-15 as an electrolyte can operate over 300 cycles at room temperature. After full charge and discharge for 5 cycles, the capacity retention reaches 48.3%. In addition, the existing PPSE-15 demonstrates excellent safety and flexibility and shows great potential in high-performance Li–O2 batteries.
研究领域:
储能
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材料科学
·
电化学
·
聚合物纳米复合材料
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电池技术
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Akkammagari Putta Rangappa,Wei Xiong,Wenhua Xue,Xinxin Lu,Yiqi Geng,Yuchao Shao,Guohan Sun,Jun Zhao
Activation of molecular O 2 on catalytic surfaces to form reactive oxygen species (ROS) is a pivotal step in catalytic reactions. In this study, we synthesized a bimetallic Zn 3 In 2 S₆ (ZIS) catalyst enriched with Pd S interfaces via a straightforward cation exchange process between Pd 2+ and Zn 2+ . These interfaces function as electron reservoirs, and Pd incorporation significantly enhances photocatalytic performance by reorganizing the electronic structure of the ZIS matrix, thereby improving charge carrier dynamics and reaction kinetics. Additionally, Pd modification optimizes O 2 adsorption strength, preventing excessive population of the π* antibonding orbital that can lead to O O bond cleavage and reduce ROS generation. Theoretical calculations reveal that monodentate adsorption of O 2 on Pd-ZIS surfaces promotes efficient photo induced electron transfer across all excited states, enabling effective ROS activation. The combination of experimental findings and theoretical analysis identified the mechanisms underlying the improved selectivity of Pd-modified ZIS catalysts. As a result, the optimized Pd-ZIS-5 photocatalyst demonstrates a high photo-oxidation performance for HMF oxidation, achieving 92.4 % conversion, 86.3 % yield, and 93.4 % selectivity–representing a 1.7-fold improvement over prismatic ZIS. Overall, this work demonstrates how Pd doping and tailored O 2 adsorption strength enhance photocatalytic processes, offering valuable insights for advanced biomass conversion and sustainable chemical production.
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Ningchao Zheng,Zhizeng Pan,Shuai Kang,Deqian Zeng,Xiangbiao Yin,Qiang Wu,Yuezhou Wei,Zhuofeng Hu
Hydrogen peroxide (H 2 O 2 ) is regarded as a promising strategy for radioactive uranium removal, due to its eco-friendliness and ability to convert free UO 2 2+ into insoluble studtite. However, the spontaneous and selective production of H 2 O 2 under ambient conditions remains challenging. This study develops a P-Ag for spontaneous O 2 activation and selective H 2 O 2 synthesis under ambient conditions. The H 2 O 2 yields of P-Ag reach 1210 µmol g −1 h −1 in air and 1876.3 µmol g −1 h −1 in O 2 , surpassing most of the recently reported catalytic systems. Importantly, the H 2 O 2 generated in situ by P-Ag achieves a high uranium removal activity (48.5) within 60 min, outperforming 23 known systems. Mechanistic studies indicate that P-Ag follows a two-step single-electron O 2 activation pathway. The electron-donating Ag sites drive the complete catalytic cycle, encompassing H 2 O/O 2 adsorption, H 2 O dissociation, and *OOH/H 2 O 2 formation, while the red phosphorus substrate serves as an electron reservoir to sustain the Ag sites. The H 2 O 2 produced reacts instantaneously with UO 2 2+ to form studtite, enabling efficient uranium removal. This study not only offers new insights into the selective synthesis of H 2 O 2 via spontaneous O 2 activation, but also proposes an eco-friendly route to mitigate environmental risks from radioactive uranium contamination.
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产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2026
·
IF 6.3
Yao Chen,Tianle Hu,Jianwei Ai,Quansheng Zhou,Xinyi Su,Yuchen Zhang,Hanchen Zhang,Shuhui Guan,Zhenfeng Bian,Hiromi Yamashita
Photocatalytic dissolution of precious metals (PMs) relies critically on the generation of specific reactive intermediates; however, the rational control of radical species in visible light remains challenging. Herein, we introduced the cyano (−CN) group into g-C3N4 (denoted as g-C3N4–CN), achieving a remarkable enhancement in the dissolution efficiency of precious metals under visible light. The −CN group not only promotes the visible-light absorption of g-C3N4–CN, but also facilitates the separation of photogenerated charges. The electron paramagnetic resonance (EPR) spectroscopy further demonstrates that g-C3N4–CN instantaneously generates superoxide radicals (O2•–) via efficient oxygen reduction while simultaneously promoting the rapid production of alkyl radicals (R•) through solvent oxidation. In contrast, pristine g-C3N4 exhibits a sluggish generation of all radical species. The distinct radical generation kinetics of g-C3N4–CN is identified as the key driver for its superior dissolution efficiency, enabling precious-metal recovery rates by 2–4 times and establishing a radical-targeted strategy for sustainable photocatalysis.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yong Liu,Mingjun Han,Jianye Liu,Yaling Huang,Yisi Liu,Wenzhang Li,Yang Liu,Jie Li
The practical implementation of Li-O 2 batteries remains constrained by three persistent challenges: sluggish oxygen redox kinetics, prohibitive costs of noble metal catalysts, and insufficient activity of non-precious alternatives. Herein, we present a novel ultralow Pt (0.25 wt%) single-atom loading Co 3 O 4 nanoneedle array catalyst (Pt 1 -Co 3 O 4 ) grown on carbon cloth via an ionic substitution strategy. This material functions as an advanced self-supporting cathode for aprotic Li-O 2 batteries. Benefiting from the surface self-reconstruction induced by Pt single-atom occupied the tetrahedral central sites of Co 3 O 4 , the electronic structure of Co 3 O 4 is modified, significantly enhancing the kinetics of both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). As a result, the Pt 1 -Co 3 O 4 cathode demonstrates excellent cycling stability and a remarkably low discharge–charge overpotential of just 0.86 V. Furthermore, the Li-O 2 battery with this cathode exhibits a high discharge-specific capacity (8.20mAh cm −2 ) and long cycling life (220 cycles, >1100 h at 0.1 mA cm −2 ), outperforming all reported Co 3 O 4 -based ORR/OER catalysts, as well as many non-noble metal catalysts, even those with significant noble metal loading. Crucially, the thin-film-like layers of discharge product Li 2 O 2 are uniformly dispersed on the Pt 1 -Co 3 O 4 nanoneedles. This reduces the adsorption energy between LiO 2 /Li 2 O 2 and Pt 1 -Co 3 O 4 compared to Co 3 O 4 , ensuring good structural stability during discharge/charge cycles and facilitating the decomposition of discharge products during recharge, thus reducing overvoltage and enhancing battery efficiency. These findings position Pt 1 -Co 3 O 4 as a promising catalyst for Li-O 2 batteries and open new avenues for the development of oxide-based single-atom catalysis.
研究领域:
材料科学
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电化学
·
能源存储与转换
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产品关联
DOI
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Yu-Le Wang,Cong Wang,Song-Hai Wu,Yong Liu,Xu Han
Although spontaneous H2O2 accumulation by sacrificial oxidation of metal disulfides (FeS2, NiS2, etc.) under oxic conditions without external electrical/photonic input has been observed, the mechanistic understanding of HCO3– on the production of H2O2 is still not clear. In this study, HCO3– apparently accelerates the production of H2O2 on NiS2, and the produced H2O2 increases from 53.85 to 90.12 μM with increasing concentrations of HCO3– from 0 to 0.5 M at pH 9.0. Electrochemical analyses indicate that HCO3– effectively mediates the 2e reduction of O2 to H2O2 on the surface of NiS2. EPR and Raman analyses rule out the primary contributions of soluble •OH and O2•– to the production of H2O2 and reveal the presence of both ≡Ni–OO• superoxo and ≡Ni–OOH peroxo on NiS2, which are important precursors for H2O2. The presence of CO3•– also indicates that HCO3– is an important H-donor during the reduction of O2 to H2O2. DFT calculations further reveal that it is thermodynamically more favorable for ≡Ni–OO• and ≡Ni–OOH to abstract H from HCO3– than from H2O to produce H2O2, confirming that HCO3– is a better H-donor than H2O to produce H2O2 via the H-abstraction pathway. This study provides insight into the importance of HCO3– on spontaneous H2O2 accumulation by sacrificial oxidation of NiS2 under oxic conditions without external electrical/photonic input.
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 5
·期 2
·544-553
·
IF 8.262
Qin Zhao,Caixia Wu,Lina Cong,Yuhang Zhang,Guiru Sun,Haiming Xie,Liqun Sun,Jia Liu
Controlling the geometric morphology and distributive location of discharge products play an important role in the reversibility and efficiency of Li–O2 batteries. This work presents novel Co2CrO4 nanospheres (CCO) prepared via a facile method, which are applied as the electrocatalysts for Li–O2 batteries. The as-prepared CCO was characterized by XRD, XPS, SEM, TEM, BET, and TG measurements. The CCO exhibited a yolk–shell microstructure, which could facilitate fast Li+ and O2 diffusion as well as possessing enough space for the discharge product deposition. In comparison to the performance of the cell without catalyst, the overpotential of the cell with CCO was apparently reduced and the cyclability significantly enhanced. Based on the experimental results and DFT calculations, direct evidence of the CCO employment being linked to the Li2O2 morphology was provided. In addition, a catalytic mechanism was proposed. Furthermore, fundamental information about the key factors and steps involved in the Li2O2 formation and decomposition was revealed. We expect that this study gives insight into the development of electrocatalysts, the selection of O2 electrode materials, and the design of O2 electrodes for Li–O2 batteries, as well as advancing our understanding of the catalytic mechanism.
研究领域:
材料科学
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电化学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Xuecheng Cao,Chaohui Wei,Xiangjun Zheng,Kai Zeng,Xin Chen,Mark H. Rummeli,Peter Strasser,Ruizhi Yang
Lithium–oxygen (Li–O 2 ) batteries have attracted tremendous attention due to their high specific energy density . However, their sluggish conversion kinetics and detrimental parasitic reactions would deteriorate the lifespan of batteries. Herein, a combined density functional theory (DFT) calculation and experimental approach is carried out to design an efficient cathode electrocatalyst for Li–O 2 batteries. A self-supporting film of Ru clusters anchored on Magnéli phase Ti 4 O 7 enriched with oxygen vacancy (Ru/Ti 4 O 7 ) is fabricated upon electrospinning and carbothermal reduction. In such a synergistic configuration of Ru/Ti 4 O 7 hybrid film, the strong metal-support interaction (SMSI) between Ru and Ti 4 O 7 can improve the charge transfer at the interface and enhance the adsorption energy of intermediates, accelerating the reaction kinetics of the formation/decomposition of Li 2 O 2 . Benefitting from this SMSI, the electrochemical stability of Ru/Ti 4 O 7 over cycling is also enhanced. As a result, as-prepared Ru/Ti 4 O 7 cathodes could realize excellent electrochemical performance , including high specific capacity (11000 mAh g –1 ), low discharge/charge polarization (0.36 V), long lifespan (> 100 cycles) and superior rate capability. Furthermore, a flexible Li–O 2 pouch cell, constructed with as-fabricated Ru/Ti 4 O 7 film cathode, lithium foil anode and GPE , can exert an impressive areal capacity of 5 mAh cm –2 with a low voltage gap of 0.82 V in ambient air. This work suggests that the activity of catalysts can be significantly enhanced with interfacial modification, offering an efficient approach for rational designing of electrocatalysts for use in Li–air batteries and beyond.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
ChemSusChem
·
2024
·
IF 7.5
Dan Li,Qian Chen,Rui Li,Yaolin Hou,Yulong Liu,Haiming Xie,Jia Liu,Jiefang Zhu
Graphical The incorporation of the polyionic liquid additive [PBVIm]-TFSI in LiI-mediated Li-O 2 batteries enables the in situ formation of a protective layer on the Li anode. [PBVIm] + cations migrate to the Li anode, forming a cationic shield that promotes uniform Li + deposition. A [PBVIm][TFSI]-containing cell demonstrates a considerable reversibility and cycling stability. Redox mediators (RMs) have shown promise in enhancing Li-O 2 battery cycling stability by reducing overpotential. However, their application is hindered by the shuttle effect, leading to RM loss and Li anode corrosion. Here, we introduce a polyionic liquid, poly (1-Butyl-3-vinylimidazolium bis(trifluoromethanesulfonylimine)) ([PBVIm]-TFSI) as an additive, showcasing a novel Li anode protection strategy for LiI-mediated Li-O 2 batteries. [PBVIm] + cations migrate to the Li anode, forming a protective cationic shield that promotes uniform Li + deposition. The addition of [PBVIm]-TFSI enhances the cycling stability, achieving 105 cycles at 200 mA⋅g −1 , compared to the cell with LiI which exhibited 38 cycles under the same conditions. Synchrotron X-ray tomography reveals the evolution of this protective layer, providing insights into its formation mechanism, in conjunction with XPS analysis. Our findings offer a new approach to Li anode protection in Li-O 2 batteries, emphasizing the critical role of interfacial engineering for battery performance.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
shuailong Song,Zhinan Wu,Tong Zhou,Yunxia Wen,Wei Cao,Han Lin,Xiaohua Lu,Tuo Ji,Jiahua Zhu
The major challenge that solid amine sorbents face in practical large-scale applications is their susceptibility to degradation under humid and oxygen-containing conditions. This study developed a superhydrophobic alkyl-silica by co-hydrolyzing alkyl-silane and tetraethyl orthosilicate and then immobilizing polyethyleneimine as a CO2 sorbent. By adjusting the chain length and density, the surface of the alkyl-silica has abundant alkyl chains, and the PEI molecules are intercalated into the surface alkyl layer. These alkyl chains effectively block the contact of O2 and H2O with the amine group, thereby selectively allowing the adsorption/desorption of CO2 molecules through the alkyl layer. The results showed that the working capacity of PEI/alkyl-silica was maintained at 86% by oxidation treatment and 85% by rinsing treatment, respectively, exhibiting excellent stability compared to unprotected PEI/SiO2. Meanwhile, the alkyl chain due to the steric hindrance effect weakens the interaction between CO2 and amine and does not reduce its original working capacity. The energy consumption of PEI/alkyl-silica during regeneration was lowered to 1.24 GJ·t-1-CO2. This interfacial building concept provides a new path for designing a long-term stable amine sorbent for cost-effective CO2 capture by avoiding the contact of O2 and H2O with the amine.
研究领域:
材料科学
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环境科学
·
化学工程
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Changshun Deng,Xiaorong Zhu,Jun Yao,Yibo Wang,Chenyang Shen,Bingqing Ge,Chaoxiang Li,Nianhua Xue,Luming Peng,Xuefeng Guo,Yan Zhu,Yafei Li,Weiping Ding
The direct oxidation of toluene by O 2 to benzaldehyde with high efficiency is a bright route for the green production of benzaldehyde but still a significant challenge. In this study, we develop a ligand modification strategy by bonding organophosphonic acid (OPA) to VTiO x /γ-Al 2 O 3 to restructure its interface microenvironment for enhancement of toluene oxidation to benzaldehyde. The as-prepared catalyst exhibits excellent selectivity over 99 % under mild conditions. Results of comprehensive characterizations and calculations reveal that the OPA bonding in bidentate with the V 6-coordinated species causes noticeable phase reconstruction between VO x and TiO 2 , thereby generating nearby new reactive oxygen species, which is responsible for the conversion of toluene to benzaldehyde at temperatures as low as ∼50 °C, much lower than that over VO x /TiO 2 (>130°C). The interface microdomain around the bonding site of OPA helps to significantly weaken the methyl C H bond of toluene molecule in reaction manifested as the significant decrease in apparent activation energy. Hence, the current work reveals a novel mechanism of the typical catalyst VO x /TiO 2 under OPA bonding, which is useful to solve the classic difficult reaction of toluene to benzaldehyde by O 2 oxidation.
研究领域:
催化化学
·
绿色化学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jiaming Wang,Feifei Kang,Yifei Chen,Xiujuan Zhang,Xiaobin Jiang,Gaohong He,Xuehua Ruan
Artificial lung membranes are the heart for extracorporeal oxygenation. Hereinto, the nonporous PDMS-based membranes have excellent biocompatibility, and also isolation ability to both blood and harmful matters. Nevertheless, their CO 2 /O 2 selectivity, in the conventional cases using pure-oxygen sweeping stream, is not enough to accomplish sufficient CO 2 removal in balance with O 2 addition. In this work, the oxygenation mode using oxygen-enriched stream, faithfully based on the permeation mechanism, is established to overcome this bottleneck. To neutralize the negative impacts caused by lowering oxygen content and its partial pressure, PDMS-based composite membranes with ultra-thin selective layer to enhance mass transfer have been fabricated successfully. The experiments manifest that the selective layer, on the basic condition that the composite structure is stable enough to make surface modification and realistic utilization, is decreased to 376 nm on the porous substrates. O 2 and CO 2 permeation rates through the ultimate membrane samples have been enhanced to 502 GPU and 4117 GPU, respectively. In this instance, the essential oxygenation could be sustained with O 2 partial pressure less than 446 mmHg in the sweeping stream. The minimum membrane area for a common treatment case is 0.05 square meters. Once the membrane area is increased to 0.18 square meters, the sterile air after purification could be directly used for oxygenation. In comparison to the oxygenation devices being used currently, membrane area can be saved by about 90 %, which is highly significant to reduce the injuring influence on blood cells. All in all, the artificial lung membranes with ultra-thin PDMS coating layer have promising future in realistic utilization.
研究领域:
生物医学工程
·
材料科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）