Sustainable Energy & Fuels
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2024
·Vol. 8
·期 8
·1730-1739
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IF 5
Caitao Kang,Chenglong Ding,Yao Li,Yanming Li,Changli Li,Jingfu He
Electrochemical CO2 reduction (CO2R) in acidic electrolytes can effectively overcome the challenge of carbonate formation and poor carbon utilization efficiency of CO2R in alkaline and neutral electrolytes. The corresponding anodic reaction design in an acidic environment therefore becomes important to overcome the valueless products and high energy consumption of the oxygen evolution reaction (OER) that hinder the overall commercial value of CO2R systems. Herein, we designed an efficient coupling system of electrochemical CO2 reduction and chlorine oxidation in an acidic electrolyte to reduce CO2 loss and improve the sustainability of the reaction system. We modulated the local microenvironment to promote C–C coupling by combining the cation effect with the larger surface area CuO nanoparticle catalyst in an acidic electrolyte. As a result, this coupling system can achieve high C2H4 and Cl2 faradaic efficiencies (FEs) of 63% and 89% at 700 mA cm−2 simultaneously. The system is commercially promising as it stably produces valuable products at both the cathode and anode.
研究领域:
电化学
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能源转化
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催化科学
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产品关联
DOI
高影响因子
Materials Science and Engineering B-Advanced Functional Solid-State Materials
·
2026
·
IF 5.7
Tao Zhang,Yugang Zhou,Wei Fang
A ZrO 2 -PSU composite membrane with asymmetric structure was developed for chlor-alkali electrolysis. • ZrO 2 addition enhanced hydrophilicity and reduced area resistance but lowered bubble point pressure. • The membrane reactor achieved high Faradaic efficiencies (>96% for HER and > 98% for CER) with considerable NaOH yield. • The zero-gap electrolyzer delivered 3.33 V at 100 mA cm −2 over 20 h with robust structural and chemical stability. The chlor-alkali process is a vital industrial route for the production of chlorine (Cl 2 ), hydrogen (H 2 ), and sodium hydroxide (NaOH). However, conventional ion-exchange membrane-based technologies face challenges related to high cost, limited durability, and susceptibility to fouling and degradation under harsh operating conditions. Here, we report a zirconium dioxide-polysulfone (ZrO 2 -PSU) composite membrane reactor that enables simultaneous and efficient Cl 2 and H 2 /NaOH production via chlor-alkali electrolysis. The composite membrane, fabricated via phase inversion tape casting, integrates ZrO 2 nanoparticles into a porous PSU matrix, achieving a well-defined asymmetric structure with a dense top layer and a finger-like porous bottom layer. The optimized composite membrane ( Z -PSU-70) exhibits lowest area resistance, enhanced hydrophilicity, and effective gas barrier properties. In an H-type electrolysis cell using a nickel mesh cathode and a RuO 2 @carbon paper anode, the reactor delivers stable cell voltages and high Faradaic efficiencies (>96% for H 2 and > 98% for Cl 2 ) with minimal gas crossover. Furthermore, a zero-gap flow cell configuration achieves a low cell voltage of approximately 3.33 V at 100 mA cm −2 , with stable performance over 20 h. Post-electrolysis characterizations confirm the structural and chemical stability of both the membrane and electrodes. This work presents a cost-effective and high-performance membrane reactor design, offering a promising pathway toward more sustainable and efficient chlor-alkali electrolysis.
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Jiejun Ye,Aqiang Chu,Yidan Zhou,Yan Xu,Shenxiang Zhang
Zinc-chlorine (Zn-Cl 2 ) battery with high discharge voltage, attractive theoretical energy density and inherently low-cost active materials provides affordable and scalable solutions for stationary energy storage. However, the Zn-Cl 2 battery suffers from rapid capacity decay and low coulombic efficiency (CE), primarily due to uncontrolled overflow of Cl 2 gas from the electrolyte. Solvents with high chlorine solubility like CCl 4 combine high chlorine storage capacity, delivering a theoretical volumetric capacity of up to 97 Ah L −1 , but at the cost of suffering from water-oil interfacial instability. In this work, we designed a wettability-tailored membrane electrode with CNT and Pt nanoparticle that stabilizes the two-phase interface and exhibits electrocatalytic activity. Moreover, leveraging the abundant and low-cost chloride in seawater, we replace deionized water with seawater. When using a seawater-based electrolyte, the Zn-Cl 2 flow battery delivers 600 stable cycles (over 220 h) with an average CE of 88.37%. Notably, it maintains 1420 stable cycles (over 544 h) at 0 °C, accompanied by an average CE of 91.94% and a capacity retention of 94.1%. This work establishes a new paradigm for the design of interface regulation strategies in Zn-Cl 2 flow batteries, providing a feasible approach for high-capacity, seawater-based energy storage systems suitable for coastal low-temperature applications.
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DOI
高影响因子
IONICS
·
2022
·Vol. 28
·期 9
·4321-4329
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IF 2.961
Zhang Jin-Zhong,Wu Shuai,Shen Fengxia,Song Wenkang,Hua Yaxin,Wu Zhenyu,Zhang Xiao-Gang,Shi Jin
A novel gas diffusion electrode (GDE) electrolyzer has been constructed to convert CO 2 into CO, with chlorine (Cl 2 ) and sodium carbonate (Na 2 CO 3 ) produced as the by-products. Using this method, the product value yielded from CO 2 electrolysis can be increased substantially. In contrast to the conventional GDE electrolyzer, we use a cation-exchange membrane as the diaphragm to separate the cathode from the anode compartment, and use NaCl aqueous solution as the anolyte. During the electrolysis process, CO 2 is reduced to CO on the cathode, with CO 3 2− generated accompanied with CO formation. On the anode, Cl − is oxidized to Cl 2 . Na + in the anode chamber transfers through the cation-exchange membrane, and migrates into the catholyte. Thus, Na 2 CO 3 can be obtained owing to the co-existing of Na + and CO 3 2− in the catholyte. Using this method, CO 3 2− penetrating through the anion-membrane can be avoided. This problem has been considered as the crucial obstacle that impedes the practical utilization of the conventional GDE electrolyzer. Our designed GDE electrolyzer has a promising application perspective in the phosgene chemical industry.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2025
·
IF 6.9
Yangyang Li,Ji Li,Ting Li,Xiaoli Cheng,Yingming Xu,Shan Gao,Lihua Huo
Chlorine (Cl 2 ), a toxic and hazardous gas with a pungent odor, has already posed threat to air quality and human health. Therefore, developing chlorine sensors with high response and low power consumption is crucial. In this work, raspberry-like SnO 2 decorated uniformly with SnS nanoparticles was synthesized via a facile solvothermal method followed by an in-situ sulfurization process, which can be used for highly selective and sensitive detection of Cl 2 at 50 °C. The SnS/SnO 2 sensor exhibits ultrahigh response (R g /R a = 1136) toward 10 ppm Cl 2 at optimal working temperature of 50 °C, achieving low detection limit down to 0.05 pp m (S = 1.52), which is 2.5 times higher than that of pure SnO 2 sensor. Its superior sensing performance can be attributed to the formation of the p-n heterostructure, which accelerates electron transfer within the material. More importantly, the as-prepared SnS/SnO 2 sensor still exhibits effective and stable detection performance toward residual chlorine in daily life, significantly extending its practical applicability and providing valuable reference for developing high-performance near room-temperature gas sensors.
研究领域:
材料科学
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气体传感技术
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纳米技术
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环境监测
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产品关联
DOI
高影响因子
WATER RESEARCH
·
2023
·
IF 12.8
Zhao Song,Yu Zhang,Xue Zhang,Xu Zhou,Yidi Chen,Xiaoguang Duan,Nanqi Ren
Peracetic acid is an emerging oxidant and disinfectant for wastewater purification. In this study, we first developed a comprehensive and accurate model to elucidate the reaction mechanisms and simulate reaction kinetics of peracetic acid (PAA, CH 3 C(=O)OOH) activated by chloride (Cl – ) based on experimental results and literature. A diversity of experiments methods (e.g., quenching experiments, probe compounds degradation, electron paramagnetic resonance (EPR) measurements) and kinetic modeling were used to determine the reactive species. As a result, carbon-centered radicals and free chlorine reactive species (Cl 2 and HClO) were devoted to BPA degradation in the PAA/Cl − system. The carbon-centered radicals CH 3 C(=O)OO • , CH 3 C(=O)O • , CH 3 OO • , and • CH 3 greatly accelerated BPA degradation with their corresponding kinetics of k CH 3 C(=O)OO•, BPA = 2 × 10 8 M − 1 s −1 , k CH 3C(= O)O• , BPA = 2 × 10 7 M − 1 s −1 , k •CH 3 , BPA = 2 × 10 6 M − 1 s −1 and k CH 3 OO•, BPA = 2 × 10 4 M − 1 s −1 . Dissolved Cl 2 (l) species was also important for BPA degradation with k Cl 2 , BPA of 2 × 10 7 M − 1 s −1 , much higher than HClO/ClO − of k HClO, BPA = 1.2 × 10 1 M − 1 s −1 and k ClO − , BPA = 9 × 10 −3 M − 1 s −1 . While free chlorine tends to transform BPA to estrogenic chlorinated organic products, the primary degradation of BPA by carbon-centered radicals results in chlorine-free products, reducing the production of disinfection byproducts during the treatment of saline wastewater. This study improves the knowledge of reaction kinetics and mechanism and reactive species generation in the PAA/Cl – system.
研究领域:
环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
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2025
·
IF 6.5
Mengshan Deng,Chaosi Liu,Jiaqi Xu,Xinqing Lu,Rui Ma,Yanghe Fu,Weidong Zhu
Rutile-type TiO 2 supported RuO 2 catalysts show a remarkably low-temperature activity in the catalytic gas-phase oxidation of HCl to Cl 2 , i.e. , the Deacon process. Although it is found that the oxygen vacancies in TiO 2 can enhance the activity and stability of supported RuO 2 catalysts in the Deacon process, the role of oxygen vacancies in the catalytic performance has not been clearly illustrated yet. In the current study, oxygen vacancies were introduced onto TiO 2 through a straightforward yet highly effective treatment of the commercial rutile-TiO 2 with H 2 at an optimal reduction temperature of 600 °C, named TiO 2 -600, which was then used as the support for preparing RuO 2 /TiO 2 -600 via an incipient wetness impregnation method. The comprehensive characterizations of TiO 2 , TiO 2 -600, and their supported RuO 2 catalysts conclusively demonstrate that the introduced oxygen vacancies on TiO 2 are consumed for the formation of the RuO 2 nanoparticles with the enhanced RuO 2 dispersion and the increased interactions between RuO 2 and TiO 2 -600, resulting in the higher catalytic activity and stability of RuO 2 /TiO 2 -600 in the Deacon process, compared to RuO 2 /TiO 2 . Consequently, this study not only clarifies the role of oxygen vacancies on TiO 2 but also offers valuable insights to guide the development of Deacon catalysts with a high low-temperature activity and a long-term stability.
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
·
IF 7.2
Shuai Wu,Xinbo Shi,Jin Shi,Tianyou Chen,Ting Jin,Fengxia Shen,Jiangfeng Mou,Shipeng Miao
A three-membrane electrolysis cell has been developed for the efficient conversion of CO 2 to CO, with Cl 2 and Na 2 CO 3 produced as byproducts. This cell consists of two chambers separated by a three-membrane assembly comprising a cation exchange membrane (CEM), a liquid electrolyte membrane (LEM), and a polyethylene (PE) membrane. In the cathodic chamber, CO 2 is electrochemically reduced to CO in organic electrolyte. And in the anodic chamber, Cl⁻ is oxidized to Cl 2 in aqueous solution. Simultaneously, Na⁺ migrates through the three-membrane system and enters into the cathode compartment, where, they combine with CO 3 2− generated from CO 2 reduction to form solid Na 2 CO 3 . The produced CO and Cl 2 can be served as feedstock for phosgene synthesis. This work presents a promising strategy for converting CO 2 into high-value chemicals.
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Sumin Wang,Rui Gao,Yuanyuan Wu,Ting Li,Ming Zheng,Xianfa Zhang,Yingming Xu,Shan Gao,Xin Zhou,Lihua Huo
Synthesizing a gas-sensitive material for detecting Cl 2 at low temperatures remains a challenge in terms of lowering the operating temperature of the gas sensors. In this paper, a simple hydrothermal method was used to prepare thin film of MIL-68(In) nanoparticles grown in-situ on ceramic tubes and calcined to obtain an oxygen defect-rich In 2 O 3 sensitive thin film. At a low temperature of 50 °C, this In 2 O 3 thin-film sensor can achieve a response of 14.1–5 ppm Cl 2 , with a minimum detectable concentration of 100 ppb. The sensor has a clear advantage in terms of optimal operating temperature. In addition, the optoelectronic properties of the sensor, the types of adsorbed oxygen on the surface and the effect of oxygen defects are investigated in detail, and the density functional theory calculations were used to corroborate the actual characterization results with the theoretical calculation simulation results. It provides an in-depth analysis of the reasons for the excellent sensing performance of the sensor to chlorine.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Quanfa Zhong,Zhong Zhang,Qinglong Fu,Jin Yu,Xiaoting Liao,Jianshu Zhao,Di He
Cl 2 •− can be the dominant radical species when high salinity wastewater is treated by advanced oxidation processes (AOPs). In this study, the steady-state concentrations of HO • , Cl • and Cl 2 •− were determined during the Fenton treatment of two landfill leachate concentrates with significantly different Cl − concentrations (XPNF: 1406 mg/L; SNNF: 8036 mg/L). Based on the steady-state concentrations of the radical species and measured second-order rate constants with dissolved organic matters (DOM), HO • accounted for 76.2% of DOM transformation in XPNF, while Cl 2 •− accounted for 96.5% in SNNF. The DOM transformation dominated by HO • or Cl 2 •− was then thoroughly compared to investigate the reactivities of HO • and Cl 2 •− with DOM at molecular level using high-resolution mass spectrometry. The results showed that formulas with low oxidation degree (O/C < 0.5) were preferentially removed by HO • and HO • was more reactive towards compounds with high saturation degree (H/C > 1.5) compared with Cl 2 •− . In contrast, Cl 2 •− was more reactive to the compounds with lower saturation level (H/C < 1.5) and the reaction of Cl 2 •− with DOM was less dependent on DOM oxidation degree. In addition, HO • preferentially reacted with the CHON compounds with low N content, while Cl 2 •− was more reactive to CHON compounds with higher N content compared with HO • . To our knowledge, this is the first study to distinguish the difference in the reactivity of HO • and Cl 2 •− towards DOM at molecular level.
研究领域:
环境科学
·
化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xiaoqian Meng,Rui Gao,Ming Zheng,Xin Zhou,Xianfa Zhang,Xiaoli Cheng,Yingming Xu,Shan Gao,Lihua Huo
Real-time monitoring of chlorine gas (Cl 2 ) with a strong irritating odor is an indispensable means of avoiding its contamination of the air and harm to the body. To achieve this purpose, a novel gas-sensitive material capable of detecting low concentrations of Cl 2 at near room temperature is developed in this paper. ZIF-8 with a kinetic diameter of 3.4 Å in the designed ZnO@ZIF-8 composites is able to sieve gas molecules with different kinetic diameters, enabling effective improvement of the selectivity of the gas-sensitive materials. In addition, the porous structure of ZIF-8 can provide more reactive sites, which is conducive to improving gas adsorption capacity and providing of channels for gas diffusion. In this study, ZnO@ZIF-8 heterojunction composites are prepared by combining the advantages of ZnO and ZIF-8, which provides a new method for real-time monitoring of low concentrations of Cl 2 , and also has potential practical applications in fields such as environmental monitoring and industrial safety.
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science and Ecotechnology
·
2021
·
IF 0
Shuang-Yang Zhao,Cheng-Xin Chen,Jie Ding,Shan-Shan Yang,Ya-Ni Zang,Xu-Dong Qin,Xin-Lei Gao,Zhao Song,Nan-Qi Ren
Chlorination has been intensively investigated for use in water disinfection and pollutant elimination due to its efficacy and convenience; however, the generation and transportation of chlorine and hypochlorite are energy-consuming and complicated. In this study, a novel binary photosensitizer consisting of anthraquinone-2-sulfonate (AQ2S) and graphene was synthesized via a π-π stack adsorption method; this compound could allow for the chlorination of organic pollutants using on-site chlorine generation. In this photosensitive degradation process, sulfapyridine (SPY) was selected as a model pollutant and was decomposed by the reactive species (Cl 2 •- , Cl • and O 2 •- ) generated during the photosensitive oxidation of chloride. The synthesized AQ2S/graphene exhibited superior activity, and the degradation rate of SPY was over 90 % after 12 h of visible light irradiation with a kinetic constant of 0.2034h −1 . Results show that 20 mg AQ2S/GR at a 21 % weight percentage of AQ2S in a pH 7 SPY solution with 1 mol/L Cl − achieved the highest kinetics rate at 0.353 h −1 . Free radical trapping experiments demonstrated that Cl 2 •- and O 2 •- were the dominant species involved in SPY decomposition under solar light. The reusability and stability of this composite were verified by conducting a cycle experiment over five successive runs. The capacity of photodegradation still remained over 90 % after these 5 runs. The current study provides an energy-efficient and simple-operational approach for water phase SPY control.
研究领域:
环境科学
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水处理
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光催化
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污染物降解
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产品关联
DOI
PubMed
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