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Journal of Physical Chemistry C · 2014 · IF 4.835

Influence of Gold Nanoparticles Anchored to Carbon Nanotubes on Formation and Decomposition of Li2O2 in Nonaqueous Li–O2 Batteries

Wugang Fan,Xiangxin Guo,Dongdong Xiao,Lin Gu

Gold nanoparticles (AuNPs) anchored to vertically aligned carbon nanotubes (VACNTs) act as additional nucleation sites for the Li2O2 growth, leading to the decreased size while increased density of Li2O2 particles in process of discharge. Correspondingly, at the deep discharge to 2.0 V the batteries show increased specific capacity. Upon charge, the AuNPs exhibit promotion effect on the Li2O2 decomposition by improving the conduction property of the discharge-formed particles, rather than by imposing the conventional electrocatalytic effect on the oxygen evolution reaction. Moreover, the AuNPs show promotion effect on decomposition of carbonate species arising from the side reactions. These effects consequently lead to the reduced charge overpotentials and extended cycle operation of the batteries. The results here provide a new as well as clear picture on the role of incorporated AuNPs in the Li2O2 formation and decomposition, which would be helpful for better understanding and constructing of high-performance air cathodes.

研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2016 · IF 5.31

Mineral transformation of structural Fe(II) hydroxides with O2, Cu(II), Cr(VI) and NO2− for enhanced arsenite sequestration

Binbin Shao,Yufan Chen,Deli Wu,Chaomeng Dai,Yalei Zhang

Structural Fe(II/III) hydroxides on the shell of nano-zerovalent iron (nZVI) are reactive sites for As(III) adsorption. Well-controlled structural Fe(II) hydroxides (SFH) is prepared to serve for As(III) removal in present study. With oxygen As(III) removal by SFH occurred efficiently but the removal efficiency was greatly reduced under anoxic conditions. The mineral transformation from SFH to lepidocrocite probably contributed to the robust removal efficiency of As(III). It is found that Cu(II), Cr(VI) and NO 2 − in aqueous solution could act as oxidants and promote the mineral transformation of SFH. A more efficient As(III) removal was therefore observed without oxygen. The removal efficiency decreased in the order O 2 /SFH   ≈   Cu(II)/SFH   >   Cr(VI)/SFH   ≈   NO 2 − /SFH at near neutral pH. The removal efficiency was less dependent on the initial pH for O 2 /SFH and Cu(II)/SFH systems than Cr(VI)/SFH and NO 2 − /SFH systems. Distribution of As on solid phases was able to describe the removal mechanism of As(III), and the results showed that the mineral transformation promoted the precipitation process and inhibited outer-sphere complexation, thus leading to enhanced As removal. With Cu(II), Cr(VI) and NO 2 − , the generation of oxidants from SFH transformation drove As(III) oxidation, and contributed to total As removal.

研究领域: 环境科学 · 化学
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SusMat · 2021 ·Vol. 1 ·期 3 ·448-457 · IF 0

A carbon dot-based total green and self-recoverable solid-state electrochemical cell fully utilizing O2/H2O redox couple

Zhaomin Chen,Xiaoqing Gu,Yutong Guo,Xin Wang,Mingwang Shao,Bin Dong,Zhenhui Kang

Electrochemical cell can overcome the inherent intermittence of the renewable energy sources, thus showing great potentials in applications ranging from electrical energy storage to future smart grid. However, the current electrochemical cells could not achieve the “total green” feature by fully utilizing the clean and abundant O 2 /H 2 O redox couples due to the enormous overpotentials for both oxygen reduction reaction (ORR) and oxygen release reaction (OER). Herein, we report a “total green” electrochemical composite film cell based on carbon dots (CDots), which can realize both ORR and OER in the acid environment. The in-air voltage generation (0.95 V, with a maximum power of 5.3 μW) relies on the multiple-electron-transfer redox chemical reaction between the two active components inside the composite film, that is, ORR/OER of CDots and the redox reaction of polyaniline (PANI) on the electrode and the resulting proton concentration gradient. Interestingly, the cell can be self-recovered at low load, recharged by adding H 2 O 2 , or electrocharged at high load. We anticipate that current study may open up new opportunities for designing and developing total-green energy storage and conversion systems for diverse applications.

研究领域: 材料科学 · 能源技术 · 环境科学
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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

Interfacial integration and roll forming of quasi-solid-state Li–O2 battery through solidification and gelation of ionic liquid

Kang-Ning Gao,Hao-Ran Wang,Ming-Hui He,Yi-Qiu Li,Zhong-Hui Cui,Ya Mao,Tao Zhang

The development of solid-state lithium-oxygen batteries is currently limited primarily by the high solid-solid interfacial resistance and the lack of efficient assembly of electrolyte and electrode. In this work, noncovalent interactions between the cations of an ammonium ionic liquid and both solid electrolytes and carbon air cathodes are introduced. The ionic liquid-based electrolytes (ILE) are solidified on Li 6·40 La 3 Zr 1·40 Ta 0·60 O 12 (LLZTO) nanoparticles and gelated by multi-wall carbon nanotubes (MWCNTs), respectively, to construct LLZTO@ILE quasi-solid-state electrolyte (QSSE) and MWCNTs-LLZTO/ILE gel cathode (GC). The QSSE exhibits a high ionic conductivity of 1.71 × 10 −3  S cm −1 at 60 °C, high Li-ion transference number of 0.56, broad electrochemical window of ~4.8 V and good thermal stability . The GC shows outstanding compatibility with QSSE. Quasi-solid-state Li–O 2 batteries are assembled by integrating QSSE and GC films with a facile roll forming method, showing a low total interfacial resistance (~87 Ω cm 2 ), and excellent reversible cycles (70 cycles) with low charge overpotential (<0.44 V) and quite high electrical energy efficiency (>70%) at 60 °C and 200 mA g −1 . A 0.12 Ah pouch-type Li–O 2 battery was achieved by this method. These results suggest that the noncovalent interactions initiated by IL cations could be an effective approach to solve the solid-solid interface issue and achieve high discharge capacity in solid-state energy storage devices.

研究领域: 材料科学 · 电化学 · 能源存储
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FUEL · 2024 · IF 6.7

Preparation of Anderson-type CoMo6-2NH2@ECOF for highly active catalysis on aerobic oxidative desulfurization of fuel under O2

Xue Lu,Jingfang Li,Liye Liang,Guangming Li

Deep desulfurization with high-efficiency is imperia for environmental demands with increasing stringent standard of sulfur content in fuels. To develop high efficiency heterogeneous catalyst for aerobic oxidative desulfurization (AODS) of fuel, an Anderson-type CoMo 6 -2NH 2 (POM) as active site, which was considered to be very effective in catalyzing the activation of O 2 , was successfully anchored on the sub-stoichiometric ECOF as a carrier by Schiff-base condensation reaction between –NH 2 groups in CoMo 6 -2NH 2 and –CHO groups in ECOF. The anchoring of CoMo 6 -2NH 2 on ECOF by covalent bond resulted in the heterogenization of CoMo 6 -2NH 2 enabled CoMo 6 -2NH 2 @ECOF to be recyclable during the AODS process. When CoMo 6 -2NH 2 @ECOF was applied as catalyst for AODS of fuel with surfactant (OTAC) under O 2 , it exhibited excellent catalytic activity with almost 100 % removal rates under 95 °C for 6 h. Moreover, the catalyst can be recycled 7 times without significant loss of catalytic activity. Further, the structure-activity relationship was investigated and the reaction mechanism of AODS of fuel was verified by ESR, XPS analysis and selective quenching experiments.

CAS / MDL: 14544-47-9 10102-40-6
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ADVANCED FUNCTIONAL MATERIALS · 2026 · IF 19.9

Janus Highly Fluorinated Ether: K+-Channel Activator or Anode Corrosion Trigger in High-Concentration Electrolytes for K–O2 Batteries?

Yu Zhong,Xiaojuan Chen,Xinyang Zhang,Lei Qin

The capacity and lifespan of superoxide-based potassium–oxygen batteries (POBs) are limited by the failure of the potassium (K) anode due to oxygen crossover. The high-concentration potassium bis(trifluoromethanesulfonyl)imide (KTFSI)/dimethoxyethane recipe enables efficient anode passivation, but its high viscosity and elevated cost necessitate the use of a highly fluorinated ether co-solvent. In this study, we elucidate the indeterminate role of fluoroether in constructing the anode passivation layer. The fluoroether participates with TFSI − anions to form a robust solid electrolyte interphase (SEI) that effectively mitigates oxygen crossover. Moreover, the fluoroether shows a Janus effect that excessive addition triggers severe K corrosion, while an optimal amount leads to a desirable SEI on the K surface. This SEI acts both as an oxygen permeation barrier and as an efficient K + -conductive channel. With a more stable environment for the K anode, a POB utilizing the KTFSI-based electrolyte delivers over 200 cycles (above 800 h) with low round-trip overpotentials and high average coulombic efficiency (98.1%) as opposed to one using the potassium hexafluorophosphate-based electrolyte that fails early. Spectroscopic analyses and theoretical simulations were utilized to elucidate the molecular-scale interactions in the electrolyte components. This study provides fundamental insights and practical strategies for the development of long-life POBs.

CAS / MDL: 406-78-0
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JOURNAL OF POLYMER SCIENCE · 2026 · IF 3.9

Dithiobenzoate-Mediated Reversible Addition-Fragmentation Chain Transfer Polymerization of Methyl Methacrylate in O2-Rarefied and Hydroxyl-Labile Dimethyl Sulfoxide

Jialong Yang,Guangqun Zhai

The effect of H 2 O 2 and H 2 O 2 -ascorbic acid (Vc) pairs on defunctionalization of 2-cyano-2-propyl dithiobenzoate (CPDB) and CPDB-mediated reversible addition-fragmentation chain transfer (RAFT) polymerization of methyl methacrylate (MMA) in dimethyl sulfoxide (DMSO) is investigated. The stability of CPDB toward H 2 O 2 is monitored by UV–vis absorption spectroscopy. CPDB is partially defunctionalized by H 2 O 2 alone and more seriously by H 2 O 2 -Vc pairs at 40°C, due to the oxidation by H 2 O 2 and the stepwise addition of DMSO-derived H 3 C· radicals. MMA greatly inhibits the defunctionalization of dithiobenzoate moieties, as both HO· and H 3 C· radicals incur oligomeric MMA-terminated alkyl radicals, which conserve the dithiobenzoate moieties of CPDB. H 2 O 2 -Vc-initiated CPDB-mediated RAFT polymerization is undertaken at 30°C and 40°C. Conversion is measured by gas chromatography, and molecular weight (MW) of PMMA is determined by gel-permeation chromatography. The processes manifest a moderately controlled fashion under optimal conditions. The products at low conversion display a multi-component composition, with high-MW PMMA consisting of 90% at least. MW of PMMA increases almost linearly with the yield and maintains a narrow distribution, but higher than the corresponding theoretical MW, owing to the partial defunctionalization of CPDB. Mass spectroscopy reveals that the irreversible termination of the intermediate radicals is the primary factor. Graphical H 2 O 2 initiated reversible addition-fragmentation chain transfer (RAFT) polymerization in dimethyl sulfoxide (DMSO) with 2-cyano-2-propyl dithiobenzoate (CPDB) as both the reducing agent and CTA. The defunctionalization of CPDB by H 2 O 2 in DMSO was observed, but methyl methacrylate significantly inhibited the defunctionalization. The CPDB-mediated RAFT polymerization was fulfilled with H 2 O 2 or H 2 O 2 -Vc pairs as the initiator. MS attributed the defunctionalization to the formation and the irreversible termination of lower-activity intermediate radicals.

CAS / MDL: 201611-85-0
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2026 · IF 12.2

Entrapped Gas Bubbles as O2 Sink and Source for Reactive Oxygen Species Production in Surface Water and Groundwater Interactions

Chang Ge,Yijie Yang,Qizheng Cai,Zheng Fang,Heng Dai,Man Tong,Songhu Yuan

Surface water–groundwater interaction zones are recognized as hotspots for reactive oxygen species (ROS) production. Entrapped gas bubbles formed due to water table fluctuations are important sinks and sources of dissolved oxygen (DO), whereas their influence on ROS production remains unknown. Here, we use column experiments to simulate surface water–groundwater interactions and quantitatively investigate the role of entrapped gas bubbles in the spatiotemporal distributions of DO and H2O2. During surface water recharge, gas bubbles act as O2 sinks, which uptake O2 from DO in the infiltrated surface water and thus restrict O2 penetration and the resultant H2O2 production. For subsequent groundwater discharge, the O2 stored in gas bubbles serves as a DO source for groundwater, which promotes H2O2 production. Cycles of groundwater discharge and surface water recharge experiments support the fact that the restriction and promotion effects induced by gas bubbles persist across recharge–discharge cycles. Reactive transport modeling reveals that the peak concentration and distribution area of H2O2 during surface water recharge decrease with the increase in the degree of gas saturation, but they increase during groundwater discharge. These findings highlight the previously overlooked dual roles of entrapped gas bubbles in ROS production and distribution under fluctuating hydrological regimes.

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CHEMICAL ENGINEERING JOURNAL · 2026 · IF 12.5

Unveiling synergistic H+/O2−/e− transport in modular triple-phase composite air electrodes for efficient reversible protonic ceramic cells

Fangjie Liu,Zaifu Gong,HaiZhao Li,Wuhui Li,Yuliang Liu,Qingjie Wang

Proposes a functional modularization strategy to fabricate BZCY-GDC-LCO electrodes. • Exhibits low polarization resistance (0.141 Ω·cm 2 ) with 216 h stable operation. • Single cell delivers 0.757 W·cm −2 (FC) and 1.182 A·cm −2 at 1.3 V (EC) at 650 °C. Efficient triple-conduction (H + /O 2− /e − ) is vital for high-performance reversible protonic ceramic cells (R-PCCs), yet the underlying transport mechanisms and their specific impacts on electrode kinetics remain elusive. In this work, we employ a “functional modularization” strategy to engineer a BaZr 0.1 Ce 0.7 Y 0.2 O 3−δ -Gd 0.1 Ce 0.9 O 1.95 -LaCoO 3 (BZCY-GDC-LCO) triple-phase composite air electrode using commercially available precursors. The synergistic effects and individual roles of the conducting species in optimizing electrochemical kinetics were systematically investigated. The optimized BZCY-GDC-LCO electrode (1:1:1 mass ratio) exhibits excellent chemical compatibility, high oxygen vacancy concentration, and a well-distributed triple-phase boundary. Consequently, it achieves a low polarization resistance of 0.141 Ω·cm 2 at 650 °C and demonstrates robust long-term stability over 216 h of operation. Single-cell tests deliver a peak power density of 0.757 W·cm −2 in fuel cell mode and a current density of 1.182 A·cm −2 at 1.3 V in electrolysis mode at 650 °C. Kinetic analysis reveals oxygen adsorption/dissociation as the rate-determining step, while excessive steam partial pressure inhibits oxygen transport via surface site passivation. This work provides a scalable design strategy for high-performance R-PCC air electrodes, demonstrating that superior performance and favorable techno-economic feasibility can be achieved using conventional materials. Download: Download high-res image (166KB) Download: Download full-size image

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SEPARATION AND PURIFICATION TECHNOLOGY · 2026 · IF 9.1

In-situ H2/O2 separation in photocatalytic water splitting by hydrogen spillover-driven hydrogen storage on Ru/WO3-MWCNTs

Mengyan Duan,Long Cao,Ni Wang,Jianxin Liu,Lulu Zhang,Jiancheng Wang

Photocatalytic water splitting is hindered by flammable H 2 /O 2 cogeneration and energy-intensive post-separation. Herein, a Ru/WO 3 -MWCNTs ternary composite is designed to address these bottlenecks via a hydrogen spillover-based strategy: direct H* storage instead of gaseous H 2 generation to achieve H 2 /O 2 separation. Photogenerated H* from Ru active sites migrate through WO 3 , then is immobilized on MWCNTs as C H bonds for hydrogen storage, enabling exclusive O 2 release during photocatalysis. This composite exhibits an oxygen evolution rate (OER) of 645.28 μmol g −1  h −1 (outperforming binary counterparts) with no detectable gaseous H₂ during irradiation, alongside a stable H₂ storage capacity of 2.23 wt%. The stored hydrogen is thermally releasable, and the entire cycle of photocatalytic water splitting (hydrogen storage with O 2 evolution) and thermal H 2 release maintains excellent cyclic stability. This work establishes hydrogen storage-aided in-situ H 2 /O 2 separation as a universal strategy for addressing the core bottlenecks in photocatalytic water splitting.

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Nanomaterials · 2026 ·Vol. 16 ·期 17 ·1055 · IF 4.8

Uniformly Dispersed Fe Clusters on Nitrogen-Doped Carbon Aerogel as a High-Performance Cathode Catalyst for Li-O2 Batteries

Hang Yu,Wenjin Song,Runxin Huang,Jiale Liu,Yanshuo Du,Di Lu,Xianxian Shi,Yufang Chen

Lithium-oxygen (Li-O2) batteries are a compelling next-generation energy storage candidate owing to their ultrahigh theoretical specific energy, but their practical deployment is critically limited by sluggish cathodic oxygen reduction/evolution kinetics, severe polarization, and poor cyclability. Here, we design a composite catalyst consisting of ultrasmall iron clusters uniformly anchored on a three-dimensional nitrogen-doped carbon aerogel (Fe@NC). The material is synthesized via bidirectional freeze-drying followed by high-temperature reduction carbonization using chitosan, cellulose nanocrystals, and zinc acetate; sublimation of zinc during pyrolysis effectively suppresses iron aggregation, yielding highly dispersed Fe0 clusters of ~10 nm while preserving the aerogel’s hierarchical porous architecture rich in pyridinic and pyrrolic N species. Electrochemical tests show that Fe@NC delivers a deep-discharge specific capacity of 18,000 mAh/g, substantially outperforming pristine carbon aerogel and commercial Ketjen black, and maintains stable cycling over 280 cycles at 500 mAh/g. Microscopic and spectroscopic analyses confirm that Fe@NC promotes uniform, fine-particle Li2O2deposition without pore blockage and enables its complete reversible decomposition upon charging, effectively mitigating electrode passivation. This work demonstrates that the synergistic combination of carbon aerogel mass-transport benefits and iron cluster catalytic activity provides a viable, scalable route to high-performance Li-O2battery cathodes.

CAS / MDL: 5970-45-6
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ACS Applied Energy Materials · 2025 · IF 5.5

Suppressing the Redox Shuttling Effect Based on the Anion Trapping Composite Separator Enhances the Performance of Li-O2 Batteries

Azhagar Samy,Raja Palani,Yi-Shiuan Wu,She-Huang Wu,Jeng-Kuei Chang,Arshid Numan,Rajan Jose,Chun-Chen Yang

Rechargeable lithium-oxygen (Li-O2) batteries are at the forefront of energy storage technology. Yet, they face critical challenges, including poor capacity, high overpotential at the oxygen cathode, inefficient lithium utilization, oxygen crossover, and the troublesome growth of lithium dendrites. This study provides an innovative solution using a graphene nanosheet (GNS) composite nickel ferrite (NiFe2O4) (NiFe2O4@GNS) catalyst and ZIF-8 particles decorated glass fiber (GF) (ZIF-8@GF) separator. Remarkably, the in situ grown ZIF-8@GF composite separator boosts higher ionic conductivity (∼2.87 × 10–3 S cm–1) and transport number (tLi+ ∼ 0.58). The modified catalyst and separator performed significantly better than the unmodified analogs in terms of specific capacity and cycling stability. In short, the device using the ZIF-8@GF separator and NiFe2O4@GNS catalyst goes up to 500 cycles without any charge polarization at 300 mA·g–1 and 500 mAh·g–1. In contrast, the corresponding cycle number for the cell with an unmodified separator even using the modified catalyst is ∼209 cycles with high charge polarization. These studies reveal that the modified separator effectively minimizes oxygen and I–/I3– redox crossover, captures anions, accelerates lithium-ion transport, and prevents the harmful intermediates (like O2– or LiO2), which can drastically degrade the organic electrolyte. Furthermore, the insulating characteristics of the ZIF-8@GF membrane deter direct electron transport to ZIF-8 nanoparticles during lithium peroxide formation, thus ensuring uninterrupted access to catalytic anion trapping sites.

研究领域: 材料科学 · 电化学
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