ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Lei Shi,Gan Wang,Jian Li,Meifen Wu,Zhaoyin Wen
The practical applications of Li–O2 batteries are hindered by the large charge polarization. Recently, the development of redox mediators (RMs) brings new hope for constructing low overpotential Li–O2 batteries. However, the “shuttle effect” of RMs causes new problems. Here, based on a low-cost and environmentally friendly biomaterial–bacterial cellulose, a sulfonation strategy was adopted to produce a functional gel polymer electrolyte for LiI-involved Li–O2 batteries. Benefiting from the high-density negatively charged sulfonate groups on the sulfonated bacterial cellulose, the functionalized gel electrolyte can produce strong electrostatic repulsion force to the negatively charged I3– ions to suppress the shuttle effect. As a result, the Li–O2 battery shows a good cycling performance with eliminated self-discharge, and the Li anode is successfully protected by the inhibition of I3– shuttling. This novel approach may provide new insights into the development of functionalized gel polymer electrolytes for Li–O2 batteries with redox mediators.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Junfang Ding,Liping Li,Haorui Zheng,Ying Zuo,Xiyang Wang,Huixia Li,Shaoqing Chen,Dan Zhang,Xingliang Xu,Guangshe Li
Nanomaterials are widely used as redox-type reaction catalysts, while reactant adsorption and O2 activation are hardly to be promoted simultaneously, restricting their applications in many important catalytic fields such as preferential CO oxidation (CO-PROX) in H2-rich stream. In this work, an interface-enhanced Co3O4–CuCoO2 nanomesh was initially synthesized by a hydrothermal process using aluminum powder as a sacrificial agent. This nanomesh is systematically characterized by powder X-ray diffraction, scanning electron microscopy, transmission electron microscopy, N2 adsorption, X-ray photoelectron spectroscopy, UV–vis absorption spectroscopy, Raman spectroscopy, X-ray absorption near-edge spectroscopy, hydrogen temperature-programmed reduction, and oxygen temperature-programmed desorption. It is demonstrated that the nanomesh possesses high-density nanopores, enabling a large number of CO adsorption sites exposed to the surface. Meanwhile, electron transfer from O2– to Co3+/Co2+ and the weakened bonding strength of Co–O bond at surfaces promoted the oxygen activation and redox ability of Co3O4. When tested as a catalyst for CO-PROX, this nanomesh with an optimized pore structure and a surface electronic structure, exhibits a strikingly high catalytic oxidation activity at low temperatures as well as a broader operation temperature window (i.e., CO conversion >99.0%, 100–200 °C) in the CO selective oxidation reaction. The present finding should be highly useful in promoting the quest for better CO-PROX catalysts, a hot topic for proton exchange membrane fuel cells and automotive vehicles.
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高影响因子
RSC Advances
·
2018
·Vol. 8
·期 41
·23397-23403
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IF 2.936
Zhuo-Liang Jiang,Jing Xie,Cong-Shan Luo,Meng-Yang Gao,Huan-Liang Guo,Mo-Han Wei,Hong-Jun Zhou,Hui Sun
The mechanism of Li–O2 batteries is based on the reactions of lithium ions and oxygen, which hold a theoretical higher energy density of approximately 3500 W h kg−1. In order to improve the practical specific capacity and cycling performance of Li–O2 batteries, a catalytically active mechanically robust air cathode is required. In this work, we synthesized a freestanding catalytic cathode with RuO2 decorated 3D web Co3O4 nanowires on nickel foam. When the specific capacity was limited at 500 mA h g−1, the RuO2–Co3O4/NiF had a stable cycling life of up to 122 times. The outstanding performance can be primarily attributed to the robust freestanding Co3O4 nanowires with RuO2 loading. The unique 3D web nanowire structure provides a large surface for Li2O2 growth and RuO2 nanoparticle loading, and the RuO2 nanoparticles help to promote the round trip deposition and decomposition of Li2O2, therefore enhancing the cycling behavior. This result indicates the superiority of RuO2–Co3O4/NiF as a freestanding highly efficient catalytic cathode for Li–O2 batteries.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 26
·期 2
·1445-1454
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IF 2.8
Wang Daiyao,Zou Jing,Cai Huahua,Huang Yixin,Li Fei,Cheng Qingfeng
Advanced oxidation processes offer effective solutions in treating wastewater from various industries. The process of alkali-activated hydrogen peroxide (H 2 O 2 ) was superior for the treatment of alkaline dye wastewater because no additional reagents were required except H 2 O 2 . However, an important and interesting phenomenon had been observed that the primary reactive species were found different for degrading organic pollutants with the process of alkali-activated H 2 O 2 . Azo dye of Orange G (OG) and triphenylmethane dye of Rhodamine B (RhB) were chosen as the target organic pollutants. The influences of various parameters on OG and RhB degradation by alkali-activated H 2 O 2 were evaluated. Furthermore, different scavengers, including ascorbic acid, methanol, t -butanol, isopropyl alcohol, furfuryl alcohol, and nitro blue tetrazolium, have been tested to identify the active species involved in dye degradation, and it was found that O 2 ·− was mainly responsible for degrading OG, while HO 2 − anion was the primary oxidant for degrading RhB.
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ACS Applied Energy Materials
·
2018
·
IF 0
Huanhuan Guo,Guangmei Hou,Jianguang Guo,Xiaohua Ren,Xiaoxin Ma,Linna Dai,Shirui Guo,Jun Lou,Jinkui Feng,Lin Zhang,Pengchao Si,Lijie Ci
Lithium–oxygen batteries (LOBs) have attracted increasing interest because of their superior theoretical specific energy. However, the stability of lithium metal anode is one of the obstacles limiting their practical applications. Here, we introduce an artificial Li3PO4 solid electrolyte interphase (SEI) film to protect the lithium anode in LOB with LiI/LiNO3/DMSO (dimethyl sulfoxide) electrolyte. The Li3PO4-protected Li anode exhibits excellent electrochemical stability during the Li stripping/plating process and leads to a relatively uniform and featureless surface in LOB after cycling. Our research demonstrates that superior electrochemical performance can be achieved in the Li–O2 battery with the synergistic combination of the DMSO-based electrolyte, the LiI redox mediator, and the Li3PO4-protected Li anode. The LOB with a Li3PO4-protected Li anode exhibits a prolonged cycling life span of 152 cycles with a fixed capacity of 1000 mA h g–1 at 2 A g–1. The results in this work provide knowledge for the development of a robust strategy for protecting the Li anode in the applications of Li–O2 batteries.
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MATERIALS LETTERS
·
2014
·
IF 2.269
Ming Yan,Yan Yan,Chao Wang,Wei Lu,Weidong Shi
In this letter, Ni 2+ doped InVO 4 nanocrystals were successfully synthesized by a simple one-pot microwave-assisted method. The energy bandgap of obtained samples can be precisely controlled by varying the Ni 2+ doping amount. The O 2 production rate of obtained Ni–InVO 4 nanocrystals is higher than that of pure InVO 4 nanocrystals under visible-light, which can be ascribed to the narrowed band gaps. The corresponding 1% doped sample N1 has the highest O 2 production rate (394 μmol/h) in all samples, which is 66% higher than the undoped sample N0.
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GREEN CHEMISTRY
·
2014
·Vol. 17
·期 1
·335-342
·
IF 6.852
Muge Niu,Yucui Hou,Shuhang Ren,Wenhua Wang,Qitian Zheng,Weize Wu
Conversion of cellulose, the most abundant biomass, shows a high selectivity to yield formic acid (FA), when oxidized by O2 in NaVO3–H2SO4 aqueous solution. This conversion involves various reactions including hydrolysis and oxidation. In this work, the relationships between these reactions were studied. There are mainly two hydrolyses and two oxidations occurring in the conversion: initial hydrolysis (from cellulose to monosaccharides) and deep hydrolysis (from monosaccharides to levulinic acid); catalytic oxidation (from monosaccharides to FA) and ordinary oxidation (from levulinic acid to acetic acid). Among these four reactions, catalytic oxidation to FA and deep hydrolysis to byproducts are competitive. The increasing rate of deep hydrolysis is faster than that of catalytic oxidation, when temperature is increased. Catalytic oxidation is promoted and deep hydrolysis is suppressed, when the O2 pressure is increased. Moreover, deep hydrolysis is promoted and catalytic oxidation is suppressed, when H2SO4 concentration is increased. The hydrolysis–oxidation pathway of this conversion was proposed. Thus, the byproducts could be inhibited, and FA-oriented transformation could be realized.
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Journal of Physical Chemistry C
·
2014
·
IF 4.835
Sujie Chang,Shigang Ruan,Erlong Wu,Weixin Huang
Oxide-on-metal particles with exposed interfaces exhibit wealthy structures and functions, but their facile synthesis remains as a challenge. Herein we report a facile O2-assisted hydrothermal method to synthesize CeO2-on-Ag particles with different CeO2 thicknesses. In this novel approach Ag particles catalyze the O2 + H2O reaction to form surface hydroxyls that induce the preferential nucleation of Ce(OH)3 on the surfaces of Ag particles, eventually forming CeO2 adlayers on Ag particles. CeO2-on-Ag particles exhibit the CeO2 thickness-dependent SERS effect in which their best SERS effect is 2 orders stronger than that of Ag particles. They also exhibit CeO2 thickness-dependent catalytic performance in CO oxidation in which the best one is as active as traditional CeO2-supported Ag catalyst. These results open up new opportunities to synthesize oxide-on-metal particles and explore their functions by tuning the oxide adlayer thickness.
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高影响因子
SOLID STATE IONICS
·
2016
·
IF 2.38
Guofeng Xu,Qingrui Xue,Jianling Li,Zhanyu Li,Xinping Li,Tianheng Yu,Jiguang Li,Xindong Wang,Feiyu Kang
Lithium-excess layered cathode materials Li[Li 0.2 Mn 0.54 − x Sm x Co 0.13 Ni 0.13 ]O 2 (x = 0, 0.01, 0.03, 0.05) with different quantities of Sm were synthesized by the coprecipitation-calcination method. The rare earth element samarium (Sm) was introduced into the structure of Li[Li 0.2 Mn 0.54 Co 0.13 Ni 0.13 ]O 2 as the replacement at Mn sites. The refinement unit cell parameters from the X-ray powder diffraction patterns illustrate the doping of Sm facilitates enlarging the lithium ions diffusion passageway space of the Li[Li 0 . 2 Mn 0.54 Co 0 . 13 Ni 0.13 ]O 2 structure. The Li[Li 0.2 Mn 0.51 Sm 0.03 Co 0.13 Ni 0.13 ]O 2 electrode presented the best electrochemistry properties. The initial discharge capacity is 287.5 mAh g − 1 and the initial coulombic efficiency increases from 81.31% to 85.34% with a constant current density of 12.5 mA g − 1 , which can be attributed to the suppression of the oxygen release from the structure at the initial charge-discharge process. The Li[Li 0·2 Mn 0.51 Sm 0.03 Co 0.13 Ni 0.13 ]O 2 electrode delivers 236.1 mAh g − 1 after 40 cycles and the capacity retention ratio is 82.12% while only 206.8 mAh g − 1 and 70.85% are obtained after 40 times of cycling for the pristine electrode. The Nyquist plots indicate that the electrical conductivity and interfacial electrochemical reaction activity increase as well.
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ADVANCED MATERIALS
·
2024
·Vol. 36
·期 31
·2404319
·
IF 27.4
Zongqiang Sun,Xiaodong Lin,Chutao Wang,Yanyan Tan,Wenjie Dou,Ajuan Hu,Jiaqing Cui,Jingmin Fan,Ruming Yuan,Mingsen Zheng,Quanfeng Dong
Lithium–oxygen (Li–O 2 ) batteries, renowned for their high theoretical energy density, have garnered significant interest as prime candidates for future electric device development. However, their actual capacity is often unsatisfactory due to the passivation of active sites by solid-phase discharge products. Optimizing the growth and storage of these products is a crucial step in advancing Li–O 2 batteries. Here, a fluorine-doped bimetallic cobalt-nickel oxide (CoNiO 2– x F x /CC) with an interlaced catalytic surface (ICS) and a corncob-like structure is proposed as an oxygen electrode. Unlike conventional oxide electrodes with a “single adsorption catalytic mechanism,” the ICS of CoNiO 2− x F x /CC offers a “competitive adsorption catalytic mechanism,” where oxygen sites facilitate oxygen conversion while fluorine sites contribute to the growth of Li 2 O 2 . This results in a change in Li 2 O 2 morphology from a surface film to toroidal particles, effectively preventing the burial of active sites. Additionally, the unique open architecture aids in the capture and release of oxygen and the formation of well-contacted Li 2 O 2 /electrode interfaces, which benefits the complete decomposition of Li 2 O 2 products. Consequently, the Li–O 2 battery with a CoNiO 2− x F x /CC cathode demonstrates a high specific capacity of up to 30923 mAh g −1 and a lifespan exceeding 580 cycles, surpassing most reported metal oxide-based cathodes.
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Journal of Cleaner Production
·
2025
·
IF 10
Mingjie Huang,Bingyuan Xu,Ke Feng,Wei Xiang,Xiaohui Wu,Yiliang Lv,Tao Zhou
Microscale zero valent iron (ZVI) is a promising material for in situ water purification through O 2 activation, but its activity is hindered by the slow electron transfer rate caused by the shielding effect of the surface passivation layer. Herein, we introduce a synergistic strategy that combines an inorganic ligand, i.e., tetrapolyphosphate (TPP), with magnetic field (MF) to boost the O 2 activation efficiency of ZVI under neutral conditions. This approach has resulted in a 4.7-fold increase in the degradation rate of diclofenac (DCF) compared to the MF-unassisted system and a remarkable 22.0-fold improvement over an analogous system with MF and EDTA. Multiphysics simulations, batch experiments, and characterizations revealed that the enhanced degradation rate was not only attributed to the elevated magnetic gradient on the ZVI surface to enrich the paramagnetic O 2 and Fe ions, but also to the functions of TPP to suppress the annihilation of •OH and reduce the redox potential of Fe 2+ /Fe 3+ . Furthermore, a synergistic mechanism between MF and TPP that facilitates the detachment of the surface-bound Fe 3+ -TPP complex into the aqueous phase, thereby regenerating the surface active sites was elucidated. This study underscores the potential of the MF-TPP synergy as an effective strategy to enhance ZVI-based Fenton-like catalysis for pollutant remediation.
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JOURNAL OF NUCLEAR MATERIALS
·
2025
·
IF 3.2
Chengyu Wang,Xiaorui Xu,Yang Tong,Wentao Zhou,Yafei Wang
Pyroprocessing of spent nuclear fuel is an important step in nuclear fuel cycle with the purpose of minimizing the radiation impact on environment and recycling useful elements. One major concern in the development of pyroprocessing is the structural material corrosion in LiCl-KCl molten salt electrolyte, which is the core component of the spent nuclear fuel reprocessing. To understand the influence of O 2- impurity on the structural material corrosion in LiCl-KCl molten salt, the study investigates the corrosion behavior of Inconel 600 alloy in LiCl-KCl molten salt containing different amounts of O 2- impurities at 500 °C by immersion corrosion experiments and electrochemical analyses.The results indicate that O 2- could accelerate the high-temperature corrosion behavior. The alloy surface developed a bilayer oxide structure following 500-hour exposure to molten salt with 3 mol% O 2- , identified as a 3.36-μm-thick outer Li 2 NiO 2 layer and a 1.11-μm-thick inner LiCrO 2 layer. Based on the corrosion behaviors of Inconel 600 alloy in LiCl-KCl molten salt with different amounts of O 2- impurities, a new O 2- affected corrosion mechanism involving the formation of dual-layer oxide films and nickel-rich particles was proposed, which could provide new insights for the corrosion study in the applications of pyroprocessing of spent nuclear fuel.
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