Journal of Environmental Sciences
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2022
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IF 6.796
Jinmin Zhao,Linghao Kong,Xingyun Hu,Xianjia Peng
Recycling strongly acidic wastewater as diluted H 2 SO 4 after contaminants contained being removed was previously proposed, however, Cl(-I), a kind of contaminant contained in strongly acidic wastewater, is difficult to remove, which severely degrades the quality of recycled H 2 SO 4 . In this study, the removal of Cl(-I) using PbO 2 was investigated and the involved mechanisms were explored. The removal efficiency of Cl(-I) reached 93.38% at 50℃ when PbO 2 /Cl(-I) mole ratio reached 2:1. The identification of reaction products shows that Cl(-I) was oxidized to Cl 2 , and PbO 2 was reduced to PbSO 4 . Cl 2 was absorbed by NaOH to form NaClO, which was used for the regeneration of PbO 2 from the generated PbSO 4 . Cl(-I) was removed through two pathways, i.e., surface oxidation and •OH radical oxidation. •OH generated by the reaction of PbO 2 and OH − plays an important role in Cl(-I) removal. The regenerated PbO 2 had excellent performance to remove Cl(-I) after six-time regeneration. This study provided an in-depth understanding on the effective removal of Cl(-I) by the oxidation method.
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CERAMICS INTERNATIONAL
·
2018
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IF 3.057
Shaohai Wu,Chengyan Liu,Zhengsen Wu,Lei Miao,Jie Gao,Xiaokai Hu,Junliang Chen,Yanyan Zheng,Xiuxia Wang,Chengjin Shen,Hengquan Yang,Xiaoyuan Zhou
SnSe 2 is regarded as an attractive thermoelectric material for its structural and chemical analogy to SnSe that is claimed with the highest ZT in single crystal. In this study, the pure and Cl-doped SnSe 2 polycrystals (3%, 6%, 9% and 12% molar Cl content) were fabricated in four steps that are hydrothermal synthesis , heating purification, diffusion doping, and spark plasma sintering . The phase structure, lamellar morphology and crystallite orientation were studied for the synthesized SnSe 2 powder and the sintered pellets. The structural evolution was traced from the SnSe 2 hexagonal plates of powders to the (001) oriented grains in pellets. The Cl doping into SnSe 2 was verified by phase composition, lattice parameter , element distribution, and chemical valance. The doped Cl increased both the carrier concentration and the mobility. The anisotropic thermoelectric properties of SnSe 2 bulk materials were investigated as functions of temperature from 50 °C to 300 °C and the doping amount, respectively. The Seebeck coefficient was less anisotropic than the electrical and thermal conduction . The grain orientation influenced the anisotropy of the electrical and thermal conductivity at a similar ratio. The power factors were less dependent on temperature with an optimum in-plane 1.06 mW m −1 K −2 and out-of-plane 0.41 mW m −1 K −2 . The highest ZT s of 0.3 were attained at 300 °C in both directions.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-8
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IF 16.6
Liu Changhao,Zhang Ningsi,Li Yang,Fan Rongli,Wang Wenjing,Feng Jianyong,Liu Chen,Wang Jiaou,Hao Weichang,Li Zhaosheng,Zou Zhigang
Durability is one prerequisite for material application. Photoelectrochemical decomposition of seawater is a promising approach to produce clean hydrogen by using solar energy, but it always faces the problem of serious Cl − corrosion. We find that the main deactivation mechanism of the photoanode is oxide surface reconstruction accompanied by the coordination of Cl − during seawater splitting, and the stability of the photoanode can be effectively improved by enhancing the metal-oxygen interaction. Taking the metastable β -Fe 2 O 3 photoanode as an example, Sn added to the lattice can enhance the M–O bonding energy and hinder the transfer of protons to lattice oxygen, thereby inhibiting excessive surface hydration and Cl − coordination. Therefore, the bare Sn/ β -Fe 2 O 3 photoanode delivers a record durability for photoelectrochemical seawater splitting over 3000 h.
研究领域:
材料科学
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光电化学
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可再生能源
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Scientific Reports
·
2025
·Vol. 15
·期 1
·1-16
·
IF 3.9
Wu Yongming,Pei Kexuan,Zhou Jiayu,Xiong Jianzhong,Liu Yu,Li Panrong,Li Fangfei,Wang Jiaqi,Liu Xiangmin,Deng Mi,Wu Chenxi
A novel substitute for perfluorooctane sulfonate (PFOS), 6:2 Chlorinated polyfluoroalkyl ether acid (6:2 Cl-PFAES, F-53B), has been widely used in the electroplating and firefighting industries, raising concerns due to increasing environmental prevalence. This study systematically investigated the adsorption characteristics of F-53B by coconut shell activated carbon (CSAC) and elucidated the underlying mechanisms through adsorption kinetics, isotherm modeling, and multi-scale characterization. Results show that the maximum adsorption capacity of CSAC for F-53B reached 261.64 mg/g, with the process best described by the pseudo-second-order kinetic model (R 2 > 0.97) and the Langmuir isotherm (R 2 > 0.94). Intraparticle diffusion modeling revealed a three-stage adsorption sequence: surface adsorption (0–2 h), pore diffusion (2–8 h), and dynamic equilibrium (8–48 h). Solution pH influenced adsorption efficiency by regulating surface charge. Under acidic conditions (pH < point of zero charge, pHzpc = 4.49), strong electrostatic interactions between protonated CSAC surfaces and anionic F-53B resulted in an 85% removal efficiency. In contrast, alkaline conditions (pH > 7) led to a 70% reduction in adsorption efficiency ( p < 0.05) due to electric repulsion. The microporous-dominated structure of CSAC (specific surface area: 857.69 m 2 /g; pore volume: 0.34 cm 3 /g) facilitated synergistic adsorption mechanisms. Oxygen-containing functional groups (C-O, -OH) promoted hydrogen bonding and hydrophobic interactions, enhancing F-53B adsorption. Besides, CSAC is optimized for emergency scenarios, it achieves 99.9% removal efficiency for 1 mg/L F-53B within 8 h at room temperature, with a maximum capacity of 261.64 mg/g; also, it maintains > 85% removal efficiency under wide pH conditions and tolerates coexisting ions (e.g., Cl − , SO 4 2− , Ca 2+ ).This study highlights the multi-mechanistic synergy of CSAC in theremoval of F-53B, providing theoretical foundations and technical insights for biochar-based remediation of emerging contaminants.
研究领域:
环境科学
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化学工程
·
水处理
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吸附技术
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材料科学
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Qiong Liu,Chengbo Bai,Die He,Xueting Wu,Yiping Wu,Rong Chen
Surface defects in semiconductors play a significant role in modulating the performance of photocatalytic reactions. However, there is still insufficient exploration regarding the influence of defects on the photocatalytic CO 2 reduction performance. In this study, we achieved controllable construction of oxygen vacancies (OVs) in BiOX (X=Cl, Br) samples through one-step solvothermal treatment in polyols by adjusting the reaction time. The introduction of OVs significantly enhanced the photocatalytic activity of BiOX (X=Cl, Br) for converting CO 2 to CO. Among all the tested BiOX (X=Cl, Br) samples with OVs, BiOCl-OV-2 and BiOBr-OV-2 samples with a moderate amount of OVs exhibited the highest CO yield of 28.51 and 15.22 μmol g cat −1 after 4 hours of irradiation, respectively. Photo-/electrochemical measurements results revealed that engineering OVs into BiOX (X=Cl, Br) effectively adjusted their electronic structure, charge density and separation; however, excessive OVs may slightly degrade their photoelectrochemical properties and thus lead to reduced photocatalytic activity. Furthermore, an appropriate amount of OV was found to enhance both CO 2 adsorption capacity and photo-generated electron reduction ability, thereby further promoting the overall efficiency of photocatalytic CO 2 conversion. Through in situ FTIR spectra analysis, we uncovered the process of photocatalytic conversion from CO 2 to CO.
研究领域:
材料科学
·
环境科学
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Materials Today
·
2025
·
IF 22
Jikai Zhang,Yi Tao,Yuxuan Ye,Haiyang Wang,Xinping Wu,Zicheng Luo,Yu Shi,Qi Zhao,Zongju Cheng,Yu Guo,Bin Li,Bo Mai,Qinyou An,Xiansheng Zhang,Zhiguo Du,Shubin Yang
Although 2D transition-metal carbides (MXenes) are usually synthesized by selective etching and chemical vapor deposition approaches, they are limited by the slow reaction kinetics, resulting in their continuous production challenging. Here, we demonstrate a bubbling chemical vapor growth (BCVG) method to continuously produce Cl-terminated MXenes by the reaction of CH 4 and TiCl 4 chemical bubbles with titanium powder in a molten salt. In the molten reaction system, titanium powder would effectively react with TiCl 4 to form highly active [TiCl 6 ] y – with low Ti Cl bond dissociation energies. The multivalent [TiCl 6 ] y – could efficiently incorporate the carbon species from CH 4 to form [Ti 6 CCl 18 ] clusters on the surface of bubbles in a low energy barrier, efficiently promoting the reaction kinetics. Subsequently, Cl-terminated MXenes were produced based on the following condensation reaction of [Ti 6 CCl 18 ] clusters. The resultant MXene (Ti 2 CCl x ) exhibits an expanded structure with strong interfacial polarization between its basal planes and the polymer matrix, delivering a good electromagnetic wave absorption performance with a minimum reflection loss (RL min ) value of –52.2 dB at a thin thickness of 2.84 mm.
研究领域:
材料科学
·
化学工程
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ACS Catalysis
·
2024
·
IF 11.3
Yang Yu,Wei Zhou,Xiaohan Zhou,Junshu Yuan,Xuewei Zhang,Lijie Wang,Jingyu Li,Xiaoxiao Meng,Fei Sun,Jihui Gao,Guangbo Zhao
Limited by the violent oxidation and corrosion environment of the oxygen evolution reaction (OER) in seawater electrolysis, the design of catalysts with high activity and stability is crucial for improving the hydrogen production performance of the electrolysis cell. Herein, we report taking advantage of corrosive Cl– in seawater to achieve rapid surface reconstruction of amorphous NiFeCoP for stable seawater splitting. The successful introduction of pulse current and P constructs Cl– adsorption active sites to optimize the d-band center and induce the formation of NiFeCo(OH). Density functional theory calculations also verified that NiFeCo(OH) has satisfactory OER activity and chlorine exclusion properties. Benefiting from the electronic structure and reaction intermediate adsorption, NiFeCo(OH) only requires 255.3 mV overpotential to reach a current density of 100 mA cm–2. Meanwhile, the assigned alkaline water electrolysis cell (NFCP || Pt/C) stably operates for 320 h in natural seawater at an industrial current density of 500 mA·cm–2 with a low voltage of 1.806 V. The seawater AEM electrolyzer (NFCP || Pt/C) achieves an improved performance of high activity (2.095 V@500 mA·cm–2) and stable operation (100 h@500 mA·cm–2) to achieve economic seawater splitting. In summary, this work proposes a fast self-reconstruction of a high-performance seawater electrocatalyst for marine hydrogen energy.
研究领域:
材料科学
·
电化学
·
可再生能源
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ENVIRONMENTAL RESEARCH
·
2026
·
IF 8.2
Pengyu Liang,Xixuan Zou,Mandi Liu,Xinhua Xu,Shuchi Zhang,Dandan Ma,Donglei Wu
Groundwater is a critical component of water resources and plays a fundamental role in maintaining ecological stability and supporting economic development. Industrial activities constitute a major source of groundwater contamination. Controlling groundwater pollution in industrial production facilities has become a key priority in environmental management. In this study, we present a high-performance ex situ electrochemical remediation system designed to treat contaminated saline (Cl–Na type) groundwater from an operational coastal chemical park. The system, optimized with a Ti/RuO 2 –IrO 2 anode and Ni cathode, achieved complete removal of ammonium nitrogen (100%) and converted 79% of total nitrogen to harmless N 2 within 45 min at a current density of 5.0 mA cm −2 . Energy consumption was as low as 1.2 kWh·m −3 . Remediation efficacy was primarily driven by in situ–generated reactive chlorine species (RCS) (e.g., Cl•, Cl 2 • - , ClO•), whose formation was significantly enhanced by the presence of bicarbonate (HCO 3 − ). Notably, the system exhibited superior removal efficiency for persistent humic acid–like dissolved organic matter (DOM) compared with biodegradable protein-like DOM, resulting in a 71% reduction in overall fluorescence intensity. The system maintained robust performance across different real groundwater samples (energy consumption: 1.2-2.1 kWh·m −3 ) and demonstrated excellent electrode stability. These results demonstrate that the technology is an economically viable and effective approach for on-site remediation of contaminated groundwater in challenging coastal industrial environments.
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POWDER TECHNOLOGY
·
2026
·
IF 5.5
Xueling Yi,Jieran Fang,Yongwei Duan,Caihua Pan,Hongzhen Li,Xiaohui Duan
Microstructure construction is an effective strategy for regulating the performance of energetic materials. Herein, CL-20@Al microspheres were fabricated by integrating porous CL-20 spherulites with Al via a rapid solvent–nonsolvent method. The results show that Al is uniformly distributed on the surface of CL-20 spherulites, and the resulting CL-20@Al microspheres possess a narrow particle size distribution, abundant nanoscale pores and enhanced dispersibility. Compared to the physical mixture, the CL-20@Al microspheres demonstrate significantly improved energy release performance, with increases of 10.4% in heat release, 33.3% in peak pressure, and 24.4% in pressurization rate. Laser ignition further reveals a 72.5% reduction in ignition delay time and a 66.8% increase in combustion rate. Meanwhile, the CL-20@Al microspheres also exhibit significantly reduced impact sensitivity compared to CL-20 spherulites. The porous structure, intimate Al/CL-20 interfacial contact, and uniform Al distribution on the porous surface collectively enhance the laser ignition and energy release of CL-20@Al microspheres.
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MACROMOLECULAR RAPID COMMUNICATIONS
·
2026
·
IF 4.1
Xinhaoran Hu,Chenyu Sun,Yang Hu,Li Yang,Cencong Wang,Quanling Yang,Chuanxi Xiong,Zhuqun Shi
Growing focus on health and quality of life is driving increasing demand for skin-like wearable sensors in human motion monitoring and healthcare. Unlike traditional e-skin, ionic skin utilizes a polymer network scaffold with mobile ions, effectively overcoming the issue of poor dispersion of conductive fillers in polymer matrices. As an ionic liquid with facile synthesis and low cost, 1-ethyl-3-methylimidazolium chloride ([EMIM]Cl) forms strong interactions with both polymers and water molecules. Cellulose is a natural polymeric material with advantages such as low cost, environmental friendliness, and renewability. 2,2,6,6-Tetramethylpiperidinyl-1-oxyl (TEMPO)-oxidized cellulose nanofibrils (TOCNs) exhibit excellent biocompatibility. In this work, the TOCN-[EMIM]Cl ionic hydrogel was formed by mixing a TOCN dispersion with [EMIM]Cl ionic liquid, followed by Ca 2 + cross-linking. By adjusting the [EMIM]Cl content from 0 to 3 wt.%, the conductivity of the TOCN-[EMIM]Cl hydrogel increased from 9.43 × 10 −5 to 4.13 × 10 −4 S cm −1 . The obtained ionic skin exhibits high transparency, with a sensitivity of 2.11 kPa −1 , rapid response/recovery times (< 50 ms), and excellent cyclic stability (> 5000 cycles). Stable and distinguishable signal outputs have been achieved for human joint movements (wrist, elbow, and knee), demonstrating significant potential in flexible wearable sensors and health monitoring applications.
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Nature Communications
·
2026
·
IF 18.1
Deng Chuyan,Zhou Yujun,Cai Xin,Zhang Xuan,Wang Yunlong,Qi Junwen,Zhu Zhigao,Yang Yue,Li Jiansheng
Electrocatalytic dehalogenation can effectively detoxify chlorinated organic pollutants (COPs) by cleaving C–Cl bonds in wastewater treatment, however, it often fails to achieve complete mineralization. In particular, the fate of the released Cl - has often been overlooked and whether they can be recycled and reutilized to facilitate pollutant degradation has remained unclear. Herein, a reduction–oxidation cascade system is constructed, in which Cl - liberated during electrocatalytic reduction is directly converted into reactive chlorine species (RCS) during the subsequent oxidation step, enabling complete mineralization of organic pollutants. Quenching experiments and electron paramagnetic resonance spectroscopy (EPR) confirm the in situ reutilization of detached Cl - . Laser scanning confocal microscopy (LSCM) visualizes the adsorption and transformation of Cl - on the electrode surface, while ab initio molecular dynamics (AIMD) calculations reveal the interfacial concentration distribution of Cl - and the energy profiles of its migration. This work establishes a cascade electrocatalytic strategy that couples reduction and oxidation, enabling chlorine reutilization and providing a sustainable pathway for the removal and resource recovery of COPs.
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Science China-Materials
·
2026
·
IF 7.7
Zheng Guiping,Li Zijian,Zhou Shizheng,Jang Haeseong,Kim Min Gyu,Qin Qing,Hou Liqiang,Liu Xien
Direct electrolysis of seawater for hydrogen production offers a vital route to circumvent freshwater limitations and advance a sustainable hydrogen economy. Herein, we present a novel catalyst design strategy based on the co-doping of Ru atoms with strong chloride affinity and Cr atoms serving as Lewis acid centers into a nickel phosphide matrix (RuCr-Ni 3 P). This material is a highly active anode for direct alkaline seawater electrolysis, offering outstanding oxygen evolution reaction (OER) selectivity and operational longevity exceeding 4000 h under industrially relevant conditions. Mechanistic investigations reveal that chloride ions are not merely detrimental impurities, but are selectively captured by Ru sites to form a dynamic Ru–Cl coordination motif. This interaction electronically modulates adjacent Ni active centers, facilitating the generation of high-valent Ni >3+ species and switching the dominant OER pathway from the lattice oxygen mechanism (LOM) to the more efficient adsorbate evolution mechanism (AEM). Simultaneously, Cr sites promote the formation of Cr–OH species, which cooperatively create a localized alkaline microenvironment favorable for OER on the high-valent Ni centers. This dual-site synergistic mechanism, wherein Ru sites regulate chloride and Ni/Cr sites drive catalysis, effectively transforms Cl − from a performance-limiting species into a chemical switch that concurrently enhances both activity and stability.
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