Journal of Environmental Sciences
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2024
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IF 5.9
Jiahui Liu,Fangyuan Dong,Yaqi Huang,Yanghe Fu,Xinqing Lu,Rui Ma,Fumin Zhang,Shuhua Wang,Weidong Zhu
Reducing the cost of RuO 2 /TiO 2 catalysts is still one of the urgent challenges in catalytic HCl oxidation. In the present work, a Ce-doped TiO 2 supported RuO 2 catalyst with a low Ru loading was developed, showing a high activity in the catalytic oxidation of HCl to Cl 2 . The results on some extensive characterizations of both Ce-doped TiO 2 carriers and their supported RuO 2 catalysts show that the doping of Ce into TiO 2 can effectively change the lattice parameters of TiO 2 to improve the dispersion of the active RuO 2 species on the carrier, which facilitates the production of surface Ru species to expose more active sites for boosting the catalytic performance even under some harsh reaction conditions. This work provides some scientific basis and technical support for chlorine recycling.
研究领域:
化学工程
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催化科学
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DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
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IF 4.464
Yajian Duan,Chaojuan Li,Yaxin Hua,Shuai Wu,Yaqing Guo,Xiaogang Zhang,Yuqi Hu,Bin Yang,Yongnian Dai,Jin Shi
A novel membrane electrolysis cell has been designed to convert CO 2 into CO in organic electrolyte, with Cl 2 produced on the anode from NaCl oxidation in aqueous solution. The obtained CO and Cl 2 can be used as the feedstock to produce phosgene. Phosgene is a widely used acylating agent in a chemical industry, which can be used as feedstock to produce numerous high-value chemicals. Through this route, CO 2 can be converted into useful chemical, with huge economic profits created in this process. Our experiment results demonstrate that CO 2 can be efficiently converted into CO in our designed electrolyzer, and NaCl can be efficiently oxidized to Cl 2 . During long-term electrolysis process, NaHCO 3 is generated and accumulated between the membrane and the cathode. This phenomenon provides clear evidence for us to better understand the mechanism of CO 2 electro-reduction in organic electrolyte.
研究领域:
化学工程
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电化学
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环境科学
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2024
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IF 8
Ting Li,Xianfa Zhang,Xiaoli Cheng,Yingming Xu,Shan Gao,Lihua Huo
It is necessary to achieve highly sensitive and low temperature detection of Cl 2 for the protection of the environment and human life and health. How to achieve sensitive detection of Cl 2 at low temperature remains a challenge. The construction of heterojunction is beneficial for promoting carrier transfer, increasing active sites, thus effectively improving sensing performance of materials. In this study, the flower sphere-like Cu 2 O/CuO composite with p-p heterojunction was obtained by using Cu-CPs as precursor followed with sintering treatment. The Cu 2 O/CuO sensor exhibits high response (S=405) to 10 ppm Cl 2 at low temperature (50 °C), the response/recovery time is 50 s/2420 s. At the same time, the Cu 2 O/CuO sensor has a low detection limit (50 ppb) and good long-term stability (60 days). The characterization results, e.g. electron paramagnetic resonance (EPR), O 2 /Cl 2 -temperature programmed desorption ( O 2 /Cl 2 -TPD), X-ray photoelectron spectroscopy (XPS) etc., reveal that oxygen vacancy effectively promotes the increase of surface adsorbed oxygen, the formation of p-p heterojunction not only modulates the electronic properties of Cu 2 O/CuO but also provides abundant adsorption sites for gas. The synergistic effect of the above factors makes Cu 2 O/CuO composite exhibit satisfactory Cl 2 sensing performance.
研究领域:
材料科学
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环境科学
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传感器技术
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Guanglu Xia,Jianhao Qiu,Shengwang Gong,Dingliang Dai,Biyao Fang,Yixin Li,Jianfeng Yao
Specific intermolecular interactions are the keys to constructing benign interfacial compatibility, which determines the activities of hybrid photocatalysts. In this study, CdS/TpPa-Cl 2 /MXene hybrids were compactly developed through the mediation of chlorine groups in TpPa-Cl 2 with MXenes and CdS. Owing to the formation of the Schottky junction between TpPa-Cl 2 and MXene and the heterojunction between TpPa-Cl 2 and CdS, as well as the close interfacial contacts among them, the photogenerated electron–hole pairs are effectively separated, which ultimately results in efficient photocatalytic activities. For visible-light-driven H 2 O 2 production in ambient air and pure water, CdS/TpPa-Cl 2 /MXene hybrids could achieve a high H 2 O 2 yield of 1005 μmol·L –1 , which is 2.5, 9.7 and 6.5 times greater than those of pure TpPa-Cl 2 , MXene and CdS, respectively. The mechanism investigation revealed that an indirect O 2 reduction pathway with ·O 2 – as an intermediate occurred for H 2 O 2 production over the CdS/TpPa-Cl 2 /MXene composites, and this two-electron O 2 reduction process was manifested as the primary way. This study provides insight into the construction of multi-component composite photocatalysts with high efficiency on the basis of covalent organic frameworks.
研究领域:
材料科学
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环境科学
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化学
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2019
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IF 7.149
Yu Lei,Shuangshuang Cheng,Na Luo,Xin Yang,Taicheng An
Cl• and Cl2•– radicals contribute to the degradation of trace organic contaminants (TrOCs) such as pharmaceutical and personal care products and endocrine-disrupting chemicals. However, little is known about their reaction rate constants and mechanisms. In this study, the reaction rate constants of Cl• and Cl2•– with 88 target compounds were determined using laser flash photolysis. Decay kinetics, product buildup kinetics, and competition kinetics were applied to track the changes in their transient spectra. Cl• exhibited quite high reactivity toward TrOCs with reaction rate constants ranging from 3.10 × 109 to 4.08 × 1010 M–1 s–1. Cl2•– was less reactive but more selective, with reaction rate constants varying from <1 × 106 to 2.78 × 109 M–1 s–1. Three QSAR models were developed, which were capable of predicting the reaction rate constants of Cl2•– with TrOCs bearing phenol, alkoxy benzene, and aniline groups. The detection of Cl•-adducts of many TrOCs suggested that Cl• addition was an important reaction mechanism. Single electron transfer (SET) predominated in reactions of Cl• with TrOCs bearing electron-rich moieties (e.g., sulfonamides), and their cation radicals were observed. Cl• might also abstract hydrogen atoms from phenolic compounds to generate phenoxyl radicals. Moreover, Cl• could react with TrOCs through multiple pathways since more than one transient intermediate was detected simultaneously. SET was the major reaction mechanism of Cl2•– reactions with TrOCs bearing phenols, alkoxy benzenes, and anilines groups. Cl2•– was found to play an important role in TrOC degradation, though it has been often neglected in previous studies. The results improve the understanding of halogen radical-involved chemistry in TrOC degradation.
研究领域:
环境化学
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化学动力学
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物理化学
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水处理技术
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有机化学
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高影响因子
ACS ES&T Water
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2025
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IF 4.3
Qiqi Wan,Yiwei Han,Ruihua Cao,Shaolan Du,Jingyi Wang,Tinglin Huang,Gang Wen
The electrochemically driven UV light-emitting diode/chlorine (UV-LED/EC-Cl2) process represents an emerging advanced oxidation technology capable of simultaneously removing microorganisms and micropollutants, making it particularly suited for decentralized water treatment in rural areas (utilized naturally occurring Cl– in water). This research systematically investigated the removal efficiency and underlying mechanisms of the UV-LED/EC-Cl2 process for the selected microorganisms (Aspergillus niger spores) and herbicides (atrazine (ATZ) and 2,4-dichlorophenoxyacetic acid (2,4-D)). The results demonstrated a significant synergistic effect in fungal spore inactivation, primarily attributed to the generation of reactive radical species, which induced severe membrane disruption and elevated intracellular reactive oxygen species levels. Furthermore, the UV-LED/EC-Cl2 process exhibited exceptional herbicide removal efficiency, achieving over 90% degradation within 37 min. The coexistence of A. niger spores reduced the herbicide degradation efficiency by approximately 10%, with the degradation products of ATZ exhibiting increased molecular weight and toxicity. Even in actual groundwater, the UV-LED/EC-Cl2 process maintained a high removal efficiency. Additionally, the electrical energy per log removal of herbicide ranged from 18.3 to 32.5 kWh/m3-log, lower than that of the standalone processes. These findings underscore the potential of the UV-LED/EC-Cl2 process as an effective and energy-efficient solution for simultaneous microorganisms and micropollutant removal in decentralized water treatment.
研究领域:
环境工程
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水处理
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高级氧化工艺
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电化学
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微生物学
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环境科学
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高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-8
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IF 14.7
Geng Shitao,Zhao Xiaoju,Xu Qiuchen,Yuan Bin,Wang Yan,Liao Meng,Ye Lei,Wang Shuo,Ouyang Zhaofeng,Wu Liang,Wang Yongyang,Ma Chenyan,Zhao Xiaojuan,Sun Hao
Rechargeable calcium (Ca) metal batteries are promising candidates for sustainable energy storage due to the abundance of Ca in Earth’s crust and the advantageous theoretical capacity and voltage of these batteries. However, the development of practical Ca metal batteries has been severely hampered by the current cathode chemistries, which limit the available energy and power densities, as well as their insufficient capacity retention and low-temperature capability. Here, we describe the rechargeable Ca/Cl 2 battery based on a reversible cathode redox reaction between CaCl 2 and Cl 2 , which is enabled by the use of lithium difluoro(oxalate)borate as a key electrolyte mediator to facilitate the dissociation and distribution of Cl-based species and Ca 2+ . Our rechargeable Ca/Cl 2 battery can deliver discharge voltages of 3 V and exhibits remarkable specific capacity (1000 mAh g −1 ) and rate capability (500 mA g −1 ). In addition, the excellent capacity retention (96.5% after 30 days) and low-temperature capability (down to 0 °C) allow us to overcome the long-standing bottleneck of rechargeable Ca metal batteries.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Nature Communications
·
2026
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IF 18.1
Qihao Liu,Guanzhong Ma,Ling Wei,Caili Zhang,Jiajun Geng,Junwei Han,Debin Kong,Linjie Zhi
Rechargeable Li | |Cl 2 batteries hold promise for low temperature storage but suffer from interfacial instability due to electrolyte decomposition, particularly at cryogenic temperatures. We identify the failure mechanism as a complex solvation chemistry involving Li + , reactive SOCl 2 , and coordinating chloroaluminates that drives parasitic reactions. Here, we demonstrate a Ternary Solvation Sheath Reconfiguration strategy using lithium trifluoromethanesulfonate to engineer the solvation structure. By leveraging strong anion-cation interactions, this approach reconfigures the coordination environment to displace solvent molecules and directs the in-situ formation of a robust, bilayered positive electrode electrolyte interphase featuring an inorganic-rich inner layer. This engineered interphase effectively suppresses electrolyte degradation and enhances charge-transfer kinetics by lowering the Li + desolvation barrier. Consequently, cells employing the Ternary Solvation Sheath Reconfiguration electrolyte sustain stable cycling at –40 °C (1000 mA g⁻ 1 ), maintaining capacity retention of 99.2% and Coulombic efficiency of 99.2% after 1100 cycles, while enabling reliable operation even at –80 °C. This work establishes a systematic framework for designing functional interphases via solvation chemistry for sustainable energy storage. Cryogenic Li | |Cl 2 batteries face severe interfacial instability. Here, authors demonstrate a solvation reconfiguration strategy to build a robust interphase, enabling stable cycling of Li | |Cl 2 batteries for over 1100 cycles at –40 °C.
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2026
·Vol. 14
·期 5
·124863
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IF 7.5
Bingliang Zhang,Cong Wang,Fuyao Tong,Meixue Chen,Xiaojuan Liu,Xifeng Shi
UV-based advanced oxidation processes (UV-AOPs) show great potential for municipal wastewater advanced treatment. Although chlor(am)ine-based UV-AOPs have been widely investigated, discrepancies in chlorinated byproduct (Cl-BP) formation and biotoxicity risks among UV/chlorine (UV/Cl 2 ), UV/chloramine (UV/NH 2 Cl), vacuum ultraviolet/ultraviolet/chlorine (VUV/UV/Cl 2 ), and VUV/UV/chloramine (VUV/UV/NH 2 Cl) processes for municipal secondary effluent treatment remain poorly understood. Herein, gas chromatography, Fourier transform ion cyclotron resonance mass spectrometry, and Vibrio fischeri were employed to reveal the formation characteristics of Cl-BPs and acute toxicity variations during these treatments. The results indicated that UV/Cl 2 process produced the highest levels of total organic chlorine (TOCl), known Cl-BPs, calculated cytotoxicity, and acute toxicity. In contrast, VUV/UV/NH 2 Cl treatment exhibited the lowest values for these parameters, with reductions of 61.3%, 96.3%, 99.7%, and 28.0% relative to UV/Cl 2 system. UV/Cl 2 treatment yielded the largest number of unknown Cl-BPs with high saturation, while VUV/UV/NH 2 Cl process generated the fewest Cl-BPs, consisting of more unsaturated CHONCl compounds. Mass difference analysis revealed that Cl 2 -based AOPs had the most precursors and precursor-product pairs, with oxygenation, chlorine substitution and addition as the principal reactions, whereas NH 2 Cl-based ones were dominated by nitrogen-related reactions. Considering Cl-BP and biotoxicity mitigation, VUV/UV/NH 2 Cl process emerges as the most promising technology for advanced treatment of municipal secondary effluent. Overall, this study provides fundamental insights and technological guidance for applying (VUV/)UV-AOPs to real municipal wastewater.
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高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
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IF 15.7
Xu Qiuchen,Tang Shanshan,Li Nachuan,Wang Yan,Zhao Xiaoju,Zhang Xiao,Geng Shitao,Yuan Bin,Wang Shuo,Ouyang Zhaofeng,Liao Meng,Ma Linlin,Shang Ming,Sun Yifan,Peng Huisheng,Sun Hao
Rechargeable sodium-chlorine (Na-Cl 2 ) batteries show great promise in grid energy storage applications due to their high electrochemical performance. However, the use of highly corrosive thionyl chloride (SOCl 2 )-based electrolytes has severely hindered their real-world applications. Here we show a non-corrosive ester (methyl dichloroacetate) as a promising alternative to SOCl 2 , which can form a non-corrosive electrolyte with aluminum chloride and sodium bis(fluorosulfonyl)imide for high-performance rechargeable Na-Cl 2 batteries. The resultant battery shows a reversible capacity of up to 1200 mAh g −1 at a current density of 100 mA g −1 calculated based on the mass of carbon with a discharge voltage of ~2.5 V, a wide temperature range from −40 to 80 °C, and long-term cycling stability of 700 cycles at −40 °C, which outperforms conventional rechargeable Na-Cl 2 batteries and state-of-the-art Na metal batteries. The electrochemical performance and safety have been further extended to fibre batteries, which realize wearable applications of rechargeable Na-Cl 2 batteries. Based on donor number and charge transfer as two key descriptors, we further propose the design principle of organic electrolytes for rechargeable Na-Cl 2 batteries, which can fully unlock the designability and sustainability of organic solvents towards practical Na-Cl 2 batteries.
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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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2023
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IF 2.8
Na Sun,Xianglian Wang,Zhanmeng Liu
In this study, electrochemically generated free chlorine (EC/Cl2) was activated by UV irradiation with a light emitting diode (LED) lamp at 275 nm to degrade acetaminophen (AAP, 2 μM) in aqueous solution. The potential at a RuO2-IrO2/Ti plate anode was set at 1.5 V vs. the Ag/AgCl electrode. Chlorine was in situ generated in the presence of Cl杴 at the anode and then it was transformed into various active species such as 晑OH and reactive chlorine species (RCS) under UV-LED irradiation. The degradation of AAP was investigated using batch tests, evaluating the influence of different experimental conditions such as NaCl concentration, phosphate buffer saline concentration, irradiation time and solution pH, keeping constant the UV-LED power and temperature. Results show that AAP could be completely degraded by the hybrid process with a high mineralization ratio (73%), and the degradation process followed a pseudo-first-order kinetics. The value of the Electric Energy per Order (EEO) = 1.272 kWh m杴3 order?, which is lower than the energy consumption of some other UV-based processes for AAP degradation. Adding 1 mM HCO3杴 ions slightly decreased the rate of AAP degradation. Luminescent bacteria experiment revealed that the acute toxicity of the reacted solution could be greatly reduced and the ecological risk was effectively abated. The scavenging assay shows that RCS plays a key role in the AAP degradation. The intermediate products were identified, and possible degradation routes were proposed. The system can advantageously replace conventional UV mercury lamp based ones in the degradation of microorganic pollutants.
研究领域:
环境科学
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水处理工程
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光催化降解
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Xin Lei,Yu Lei,Shuangshuang Cheng,Xin Yang
N -nitrosamines are great concern in potable water reuse. This study investigated the reaction kinetics of chlorine radicals (Cl • and Cl 2 •− ) with N -nitrosamines. The second-order reaction rate constants of Cl • ( k Cl • ) and Cl 2 •− ( k Cl2 •− ) with eight N -nitrosamines at pH 7.0 varied in the range of (5.02 ± 0.41)–(57.1 ± 4.25) × 10 8 M −1 s −1 and (0.46 ± 0.04)–(10.6 ± 0.73) × 10 8 M −1 s −1 , respectively. The numbers of methylene groups (#−CH 2 −) showed a good positive correlation with k Cl • (R 2 = 0.71), but not with k Cl2 •− . The degradation of eight N -nitrosamines under UV/chlorine advanced oxidation process (AOP) slightly increased by 1–18% in contrast to UV irradiation alone, and Cl − in the AOPs cannot inhibit their removal. The results improved the understanding of the fate of N -nitrosamines in chlorine radical-involved AOPs.
研究领域:
环境化学
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水处理
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高级氧化过程
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DOI
高影响因子