ChemSusChem
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2024
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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
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能源存储
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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
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化学工程
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DOI
高影响因子
TALANTA
·
2024
·
IF 5.6
Yucheng Zhou,Chaoyan Zhang,Jiyang Liu,Yiping Mou
Sensitive detection of tumor biomarkers is of great significance for early cancer diagnosis, treatment evaluation, and recurrence monitoring. Development of convenient electrochemiluminescence (ECL) immunosensor using dissolved oxygen (O 2 ) as an endogenous co-reactant of luminol combined with efficient nanocatalysts to boost ECL signal in neutral media is highly desirable. Herein, sensitive detection of tumor biomarker using ECL of luminal-O 2 enhanced by confinement of nitrogen-doped graphene quantum dots (N-GQDs) and platinum nanoparticles (PtNPs) on nanochannel array was demonstrated. A high-density nanochannel array-modified electrode was achieved by rapidly growing an amino-functionalized vertically-ordered mesoporous silica film (NH 2 -VMSF) on the inexpensive and readily available indium tin oxide (ITO) electrode. Through simple electrodeposition, N-GQDs were confined and PtNPs were in-situ synthesized in nanochannels of NH 2 -VMSF. These confined nanocomposites catalyzed the electroreduction of O 2 at negative potentials to generate a large amount of reactive oxygen species (ROS) and facilitated luminol oxidation, enhancing the ECL signal of luminol by 25 times. Two immunosensors were fabricated after covalent immobilization of the recognition antibody of carbohydrate antigen 199 (CA199) or carbohydrate antigen 125 (CA125) on the outer surface of the NH 2 -VMSF and blocking of non-specific sites. When tumor biomarkers bind to the corresponding antibodies on the recognition interface, the formed immunocomplex hindered the diffusion of luminol to the underlying electrode, resulting in a decrease in the ECL signal and sensitive detection of tumor biomarker. The constructed CA199 immunosensor exhibited a linear detection range for CA199 from 0.5 mU mL −1 to 50 U mL −1 , with a detection limit (DL) of 0.03 mU mL −1 . For CA125 detection, linear detection ranged from 0.5 mU mL −1 to 500 U mL −1 , with a DL of 0.005 mU mL −1 . The fabricated immunosensors demonstrated good selectivity and high reproducibility. This study provides great potential for the development of efficient luminol ECL systems in neutral media and expands the biological application in sensitive detection of tumor biomarker.
研究领域:
生物医学工程
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分析化学
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癌症诊断
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DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2026
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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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高影响因子
AICHE JOURNAL
·
2026
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IF 4
Zhiheng Wang,Ningning Wu,Jiali Huang,Tuo Ji,Han Lin,Liwen Mu,Xiaohua Lu,Jiahua Zhu
Direct synthesis of hydrogen peroxide (DSHP) from H 2 and O 2 is indeed a promising sustainable alternative to the conventional anthraquinone oxidation process, yet achieving high H 2 O 2 productivity and selectivity simultaneously remains a significant challenge. Herein, we designed a diode-inspired interfacial microenvironment to address this challenge by synchronizing the kinetic relay of the key transport and reaction steps in DSHP. Specifically, this microenvironment was fabricated by grafting hydrophobic silane molecules onto the carbon surface followed by loading palladium nanoparticles. Results indicate that the interfacial microenvironment enables an efficient relay of H 2 dissociation, H 2 O 2 formation and desorption, shutting down the reverse path of the side reaction. Benefiting from this diode-inspired interfacial design, high H 2 O 2 productivity of 21,647.1 mol kg Pd −1 h −1 and H 2 O 2 selectivity of 93.3% were successfully achieved under ambient conditions. This work demonstrated the critical role of the interfacial microenvironment in regulating the synergy between mass transfer and reaction in heterogeneous reaction.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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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
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能源存储与转换
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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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PubMed
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
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能源科学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Tie Liu
The geometric design of atomically dispersed 'framework-active sites' grafted with carbonaceous materials to establish a well-connected three-dimensional network represents a compelling strategy for enhancing the performance of lithium-oxygen batteries, particularly in terms of cyclability. This paper introduces a simple approach that utilizes self-assembly heterogeneous nucleation to fabricate discrete bimetallic (Co, Ni) micron lattices grafted onto CNTs, exhibiting commendable surface properties. This intriguing hierarchical structure optimally harnesses the profound structural effects of CNTs weaving matrix, thereby imparting essential properties to the cathode, including high catalytic activity, intrinsically accessible active sites, and continuous porosity to accommodate discharge products. And such binary metal-nitride grafted configuration is significant in mitigating the embarrassing presence of nitrides (low conductivity) and carbon material (inferior activity). Consequently, cell measurement results indicate that a comparable capacity of 8599.7 mA h g⁻¹ and cyclic performance exceeding 200 cycles are achieved in a semi-solid state battery, outperforming commercially available RuC catalysts. And the DFT calculations further demonstrate the strong electronic coupling transfer and exceptional bifunctional activity observed in this binary metal-nitride sample. Therefore, this work exemplifies both steerable preparation techniques and the considerable potential inherent in geometric design for bimetallic sites grafted with carbonaceous material-based catalysts as they transition from Li-O 2 to Li-air batteries.
研究领域:
材料科学
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电化学
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纳米技术
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
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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
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电化学
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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
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2026
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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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高影响因子
Advanced Materials Interfaces
·
2017
·Vol. 4
·期 23
·1700693
·
IF 4.279
Kailiang Liu,Hongguang Sun,Shanmu Dong,Chenglong Lu,Yang Li,Junmei Cheng,Jianjun Zhang,Xiaogang Wang,Xiao Chen,Guanglei Cui
The increasing interest in Li–O 2 battery arises from its unparalleled theoretical energy density. Nevertheless, the poor reversibility of cathode reaction and unstable characteristic of Li anode hinder its further application. To address these issues, a high-performance sandwich-structured quasisolid polymer electrolyte (QSPE) is designed to meet the requirement of both cathode and anode. For the first time, lithiated Nafion ionomer (Li-Nafion) is introduced into Li–O 2 cell to separate “catholyte” and “anolyte.” Redox mediator (RM) is introduced into gel-like catholyte, based on polymethymethacrylate, to achieve high capacity and reversibility. Polypropylene carbonate is chosen as solid-state anolyte for enhancing interface stability of lithium anode. It is demonstrated that the QSPE exhibits excellent permselectivity to block RM shuttling, as well as good ionic conductivity and high electrochemical window. A solution mechanism formation of discharge product is demonstrated in the Li–O 2 cell with QSPE and the RM works well for cycles at room temperature. This sandwich-structured design strategy will provide a new pathway to promote the properties of Li–O 2 battery.
研究领域:
储能
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电化学
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材料科学
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电池技术
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DOI
高影响因子
危险品化学品经营许可证（带存储）