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Identifying the active sites in C-N codoped TiO_(2) electrode for electrocatalytic water oxidation to produce H_(2)O_(2)

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Journal of Central South University 2022年第9期29卷 3016-3029页

作者： XUE Sheng-guo TANG Lu TANG Tian ZHANG Feng LYU Hua-gang LIU Hong-yu JIANG Jun HUANG Yan-hong School of Metallurgy and Environment Central South UniversityChangsha 410083China Chinese National Engineering Research Center for Control&Treatment of Heavy Metal Pollution Central South UniversityChangsha 410083China Anhui Province Key Laboratory of Advanced Catalytic Materials and Reaction Engineering School of Chemistry and Chemical EngineeringHefei University of TechnologyHefei 230009China Guangxi Research Institute of Environmental Protection Nanning 530000China

Unveiling the active site of an electrocatalyst is fundamental for the development of efficient electrode *** the two-electron water oxidation to produce H_(2)O_(2),competitive reactions,including four-and one-electron water oxidation and surface reconstruction derived from the high-oxidative environment co-existed,leading to great challenges to identify the real active sites on the *** this work,Ti/TiO_(2)-based electrodes calcined under air,nitrogen,or urea atmospheres were selected as electrocatalysts for two-electron water *** analyses were applied to evaluate the catalytic activity and *** morphological and current change on the electrode surface were determined by scanning electrochemical microscopy,while the chemical and valence evolutions with depth distributions were tested by XPS combined with cluster argon ion *** results demonstrated that Ti/TiO_(2) nanotube arrays served as the support,while the functional groups of carbonyl groups and pyrrolic nitrogen derived from the co-pyrolysis with urea were the active sites for the H_(2)O_(2) *** finding provided a new horizon to design efficient catalysts for H_(2)O_(2) production.

关键词： hydrogen peroxide in-situ characterization titanium dioxide electrode carbonyl pyrrolic nitrogen

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Evolutional Solid Phase and Solid-Liquid Interface Uranium Immobilization Mechanisms by Nanoscale Zero-Valent Iron and Enhanced Uranium Stability control Strategy

SSRN

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SSRN 2022年

作者： Hua, Yilong Li, Donghan Zou, Jinglan Wang, Wei Wu, Xiaoyan Zhang, Xiaowen Liu, Qing Zhao, Guodong Li, Mi Zhang, Wei-Xian Yang, Jianping School of Resource Environment and Safety Engineering University of South China Hunan Hengyang421001 China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and Engineering Donghua University Shanghai201620 China United Laboratory of Heavy Metal Pollution Control and Resource Reuse University of South China Hunan Hengyang421001 China Hunan Key Laboratory of Pollution Control and Resource Reuse University of South China Hunan Hengyang421001 China State Key Laboratory of Pollution Control College of Environmental Science and Engineering Tongji University Shanghai200092 China

Uranium is a carbon dioxide free nuclear energy, and uranium-contained wastewater poses serious chronic health effects toward human. Nanoscale zero-valent iron (nZVI) separates uranium from wastewater with ultrafast kinetic, high capacity and selectivity. However, the dynamic interfacial uranium binding mechanisms and its stability, controlled by the phase transformation of nZVI, is important but poorly understood. After a long-term reaction, the fresh nZVI was oxidized and transfromed to ferrihydrite and then lepidocrocite and hematite. Analysis for the structures and valence states of U, Fe species indicated that the dominate U(VI) uptake mechanism changed from Fe 0 induced reduction to adsorption as nZVI transformed to iron (oxyhydr)oxides. Density functional theory calculation revealed that uranyl formed corner-sharing configurations on the surface of iron nanoparticles, and some uranium ions prefer to incorporate into the structure of lepidocrocite than hematite during the crystallization processes of ferrihydrite. Meanwhile, 100~10000 μg/L uranyl ions were quickly captured, the residual uranium could be maintained at ~9.31 μg/L and the content of uranium in reacted iron nanoparticles reached ~24.16 wt%. Interestingly, the oxidization reduction potential (E h ) was a potential parameter to control uranium immobilization in the CSTR system, and the E h control strategy could be used to increase the fraction of U(IV)/U(V), sparingly soluble and highly stable, higher than 90%. The findings augment our understanding of U-nZVI reactions and guide nZVI technology to remedy real uranium-contained wastewater. © 2022, The Authors. All rights reserved.

关键词： Hematite

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Revealing the Mechanisms of Well Iron Clogging in Groundwater Heat Pump Systems: Insights from Video Imaging, Hydro-Geo-Chemical Analysis, and Geochemical Modeling

SSRN

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SSRN 2024年

作者： Shi, Min Yang, Yuesuo Lu, Ying Wu, Yuhui Wang, Qiandan Gao, Cuiping Gao, Lei Ministry of Education Changchun130021 China Jilin Provincial Key Laboratory of Water Resources and Environment Jilin University Changchun130021 China Guangdong Engineering Technology Research Center of Heavy Metal Pollution Control and Restoration in Farmland Soil South China Institute of Environmental Sciences MEE Guangzhou510535 China Ministry of Education Shenyang110044 China Waite Campus UrrbraeSA5064 Australia

Groundwater heat pump (GWHP) systems are increasingly popular as low-carbon and environmentally friendly technologies, but well clogging induced by iron remains a significant issue. This study investigated the clogging characteristics and biogeochemistry of three typical wells (pumping, injection, and observation wells) in an operating GWHP system using video imaging, sampling, and analysis of hydro-geo-chemical and microbial data. The results revealed that iron-induced well clogging is a complex process involving physical, chemical, and microbial factors. Pumping wells experience clogging due to water mixing with varying redox conditions, resulting in hematite-based iron oxide deposits. Injection wells exhibit higher clogging severity, with transformed oxidation and accumulation of reduced iron minerals at the solid-liquid interface, resulting in darker colored clogs with magnetite. Clogging in both extraction and injection wells is closely related to iron-rich aquifer sections, where severe clogging occurs. Shallow clogging due to iron oxide is limited and attributed to the oxidation of zero-valent iron in well casing material. Iron-oxidizing bacteria and iron-reducing bacteria were detected in the consolidated deposits of clogged wells, indicating their involvement in the clogging formation process. Moreover, a strong correlation was observed between the presence of nitrate-reducing bacteria in the water phase and the severity of clogging, suggesting a possible link between iron oxidation and nitrate reduction in the system. Geochemical modeling results further supported the observed clogging severity in GWHP systems and confirmed varying clogging mechanisms in different wells and depths. These findings contribute to the understanding of clogging in GWHP operations, aiding in robust water utilization and energy-saving efforts, and supporting global carbon reduction initiatives. © 2024, The Authors. All rights reserved.

关键词： Aquifers

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Frontiers and Innovative Development of metallurgical Engineering Science and Technology in China Toward 2040

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Strategic Study of CAE 2024年第5期26卷 24-36页

作者： Chai, Liyuan Wang, Haiying Min, Xiaobo Liu, Hui Wang, Qingwei Gu, Huangling School of Metallurgy and Environment Central South University Changsha410083 China State Key Laboratory of Advanced Metallurgy for Non-ferrous Metals Changsha410083 China Chinese National Engineering Research Centre for Control & Treatment of Heavy Metal Pollution Changsha410083 China

Promoting the low-carbon and intelligent development of the metallurgical industry and establishing a low-carbon metallurgical industry system are crucial for ensuring national metal resource and energy security, strengthening the manufacturing sector, and supporting carbon reduction and ecological construction in China. Based on a global perspective, the metallurgical industry of China is still at a stage of low-end manufacturing. Therefore, it is necessary to conduct the top-level design to boost China’s strength in metallurgical development, integrating the independent control of metal resources, intelligent manufacturing, environmental protection, and national security maintenance as an organic whole. This study summarizes the frontiers and development trends of metallurgical engineering science and technology worldwide, analyzes the development vision of metallurgical engineering science and technology in China, and proposes medium- and long-term strategic measures for China’s metallurgical engineering technology development toward 2040, involving general development ideas, key strategic tasks, and main technology development directions. Furthermore, the following countermeasures are proposed: (1) developing disruptive technologies in the metallurgical field in advance, (2) integrating the industrial and innovation chains of the metallurgical industry, (3) building a sophisticated talent system, (4) improving the policy and standards systems, and (5) constructing driving forces for core technology development. © 2024 Beijing Zhongguo Gongcheng Kexue Zazhishe. All rights reserved.

关键词： Pyrometallurgy

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Simultaneous Removal of Phosphorus and Organic Contaminants from Phosphogypsum Using Hydrothermal Method for Gypsum Resource Regeneration

SSRN

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SSRN 2022年

作者： Li, Jie Peng, Xiaoqian Zheng, Jiayi Mao, Minlin Sun, Xing Wang, Jiaxin Li, Xiaoqin Chai, Xilin Lin, Zhang Liu, Weizhen School of Environment and Energy Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling South China University of Technology Guangdong Guangzhou510006 China Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution School of Metallurgy and Environment Central South University Hunan Changsha410083 China The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of Education Guangdong Guangzhou510006 China Jiangxi Gaiya Environm Sci & Technol Co. Ltd Jiangxi Shangrao334000 China

Phosphogypsum(PG) has accumulated 600 million tons in China. The biggest challenge for the utilization of PG is thorough removal of multiple contaminants, especially phosphorus and organic matter. This work investigated the speciation of phosphorus and organic contaminants in PG by FTIR spectroscopy, Raman spectroscopy, XRD, SEM-EDS and GC-MS. Under optimal hydrothermal conditions(0.3 M K 2 S 2 O 8 , heated at 120°C for 12 h), PG was transformed into anhydrous calcium sulfate powder. The whiteness significantly improved from 40.9 to 97, and the removal rate of phosphorus and organic matter reached 76% and 80% respectively. The residual phosphorus was only 0.108%, which met the standard of PG as a building material in China (P content © 2022, The Authors. All rights reserved.

关键词： Gypsum

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A Bifunctional Nitrogen-Doped Hierarchical Porous Graphite Carbon for Adsorption and Catalytic Removal of Tetracycline Antibiotics: Performance and Nonradical Mechanism

SSRN

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SSRN 2022年

作者： Pi, Zhoujie Hou, Kunjie Yao, Fubing He, Li Chen, Shengjie Fu, Yukui Li, Xiaoming Yang, Qi College of Environmental Science and Engineering Hunan University Changsha410082 China Key Laboratory of Environmental Biology and Pollution Control Hunan University Ministry of Education Changsha410082 China School of Metallurgy and Environment Central South University Changsha410083 China Chinese National Engineering Research Center for Control and Treatment of Heavy Metal Pollution Changsha410083 China

A nitrogen(N)-doped hierarchical porous graphite carbon (NHC) was synthesized at different hydrothermal carbonization temperature (400, 600 and 800°C) using a template-free and solvent-free method. The as-prepared materials possessed perfect bifunctional performance for antibiotics tetracycline (TC) removal via synergistic adsorption and catalytic degradation process. The carbonization temperature had a significant effect in the material structure and property adjustment. The carbonaceous material prepared at 800°C (NHC-800) showed optimal adsorption and catalytic oxidation efficiency for TC removal with 451.62 mg/g maximum adsorption capacity and 69.5% mineralization rate within 180 min. The rate constant for NHC-800 (0.0406 min -1 ) was 111.54-folders higher than NHC-400 (3.6400 × 10 -4 min -1 ). Moreover, the NHC-800/peroxydisulfate (PDS) system showed a good anti-interference ability to pH, inorganic anions and humic acid. The investigation of catalytic mechanisms revealed that the nonradical process governed PDS activation process using defective edges, C=O, graphitic N and pyridinic N as the active redox sites, while the large surface area of NHC-800 or the activated C (+) supported the adsorption of pollutants or PDS, further facilitated the electron-transfer process. Finally, the possible degradation pathway was proposed and the acute toxicity of the degradation intermediates was assessed. This study not only provides a facile rote for the synthesis carbonaceous materials, but also gives a detailed insight in N species and other reactive sites of carbonaceous materials in adsorption and catalytic degradation process. © 2022, The Authors. All rights reserved.

关键词： Doping (additives)

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Biohybrids Of Twinning Cd0.8zn0.2s Nanoparticles and Sporomusa Ovata For Efficient Solar-Driven Reduction Of Co2 To Acetate

SSRN

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SSRN 2023年

作者： Zhang, Kejing Li, Ruijie Chen, Jianxin Chai, Liyuan Lin, Zhang Zou, Long Shi, Yan School of Metallurgy and Environment Central South University Changsha410083 China State Key Laboratory of Advanced Metallurgy for Non-ferrous Metals Changsha410083 China Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution Changsha410083 China College of Life Sciences Jiangxi Normal University Nanchang330022 China

Integration of microorganisms with semiconductors is an effective approach to sustainable solar-driven production of chemicals from CO2, which lies in the development of efficient, highly biocompatible, and low-cost photocatalysts. Herein, twinning Cd0.8Zn0.2S nanoparticles were synthesized and used for the first time in construction of a biohybrid system (Cd0.8Zn0.2S/S. ovata) with a non-photosynthetic acetogenic bacterium of Sporomusa ovata. The Cd0.8Zn0.2S/S. ovata yielded 49.33±3.54 mM of acetate at a production rate of 8.22±0.59 mM d-1 with a quantum efficiency of 16.82±1.21 %, which exceeded those of other reported biohybrid systems. Further investigation revealed that the twin-induced homojunctions with staggered phase alignment contributed to enhancing the separation efficiency of photogenerated electron-hole pairs and avoiding the photocorrosion. Due to the dual advantages of light absorption and biocompatibility of Cd0.8Zn0.2S, the Cd0.8Zn0.2S/S. ovata could efficiently harvest light energy and transfer photogenerated electrons to cellular metabolism, driving the Wood-Ljungdahl pathway to efficiently synthesize acetate with CO2. © 2023, The Authors. All rights reserved.

关键词： Nanoparticles

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Opening New Pathways: Utilizing Liquid Passivation Agents for Cd Passivation in Soil and Mitigating Cd Accumulation in Wheat

SSRN

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SSRN 2024年

作者： Zhao, Lijie Zhang, Li Zhang, Qian Zeng, Qiang Zhao, Nan Yang, Jing Zhao, Chuanfang La, Yuepeng Lin, Dasong Wang, Ruigang Innovation Team of Remediation for Heavy Metal Contaminated Farmlands Agro-Environmental Protection Institute Ministry of Agriculture and Rural Affairs Tianjin300191 China National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in South China Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and Management Institute of Eco-environmental and Soil Sciences Guangdong Academy of Sciences Guangzhou510650 China College of Land and Environment Shenyang Agricultural University Shenyang110065 China Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing100085 China

Solid passivators, a widely application materials in Cd-polluted soils, still exists the problems of complex preparation procedures, inconvenient application and high cost. Using liquid passivators has the potential to overcome these drawbacks, but there were no reports for Cd-passivation by using liquid agents. In this study, 3-mercaptopropyltrimethoxysilanea (L-MPTMS) was firstly adopted as liquid passivator to explore its feasibility for inhibiting Cd accumulation in wheat. The density functional theory (DFT) and characterization results proved that L-MPTMS reacted with Cd to form monodentate (Cd-S) and bidentate (S-Cd-S) complex structures, which were the major reasons for the decrease of Cd availability. In the soil incubation experiment, L-MPTMS (0.025%-0.2%) notably reduced the Cd availability (9.01%-65.58%) in acid and alkaline soils from six different regions and exhibited high remediation efficiency. The pot experiment demonstrated that the application of 0.025%-0.2% L-MPTMS decreased the concentration of Cd in wheat root (11.3%-70.2%) and shoot (11.7-67.6%) and increased micronutrient Mn concentration (14.3%-40.9%) in wheat root. The biomass of wheat seedlings was elevated by 5.83%-16.94% using 0.025%-0.2% L-MPTMS. Moreover, L-MPTMS enriched Cd-immobilizing bacteria and plant growth-promoting rhizobacteria and strengthened the metabolic functions of some bacteria in soils. In the one-year wheat field trial, 0.025%-0.2% L-MPTMS significantly decreased Cd concentration in edible parts (42.47%-56.24%). These findings revealed that L-MPTMS is a promising Cd passivator for soil remediation and wheat safety production, and further indicated that liquid passivators showed excellent potential to heavy metals stabilization in soil. © 2024, The Authors. All rights reserved.

关键词： Soils

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A sensitive method for rapid determination of 256 semi-volatile organic compounds (SVOCs) in water by solid-phase extraction and GC-MS/MS

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Journal of Environmental Sciences 2025年

作者： Youchang Zhu Ruohan Sun Yanran Dong Yan Liu Yupeng Chen Zhiquan Yuan Baozhu Pan Nan Xu Key Laboratory for Heavy Metal Pollution Control and Reutilization School of Environment and Energy Peking University Shenzhen Graduate School Shenzhen 518055 China Agilent Technologies (China) Co. Ltd. Guangzhou 510630 China State Key Laboratory of Eco-hydraulic in Northwest Arid Region of China Xi'an University of Technology Xi'an 710048 China

A trace analytical method based on solid-phase extraction gas chromatography-tandem mass spectrometry (SPE-GC-MS/MS) was developed for the rapid detection of 256 semi-volatile organic compounds (SVOCs), including 25 polycyclic aromatic hydrocarbons (PAHs), 70 polychlorinated biphenyls (PCBs), 123 pesticides, 20 phthalate esters (PAEs), 4 organophosphate esters (OPEs), 9 synthetic musks (SMs), and 5 UV filters (UVs) in water. Notably, this method provided a decent linearity of calibration standards ( R 2 > 0.999), excellent method limits of quantification (MLOQs) (0.12-11.41 ng/L), satisfactory matrix spiking recovery rates (60.4 %-126 %), and high precision (intra-day relative standard deviations (RSDs): 1.0 %-10.0 %, inter-day RSDs: 3.0 %-15.0 %, and inter-week RSDs: 3.4 %-15.7 %), making it suitable for trace-level studies. Statistical analysis revealed that SVOCs with higher volatility exhibited enhanced recovery rates. Validation of the methodology involved analyzing SVOCs in real spring water and river water samples. Twenty-seven SVOCs were detected in spring water and 58 in river water, with an average concentration of 631.73 and 16,095 ng/L, respectively. Among the detected SVOCs, PAEs constituted the predominant proportion. This study underscored the presence of SVOCs contamination specifically within the spring water, although SVOCs concentrations in river water were significantly greater than those found in spring water. In summary, this sensitive method based on SPE-GC-MS/MS was successfully developed and validated for the rapid analysis of a diverse array of 256 SVOCs at trace levels in water, including not only the traditional highly valued PAHs, PCBs, pesticides, and PAEs, but also the emerging OPEs, UVs, and SMs.

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Integrated Influence of Sulfide Modification on the Reactivity of Nanoscale Zero-Valent Iron Under an Electromagnetic Field

SSRN

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SSRN 2023年

作者： Yu, Kai Tu, Yuxuan Wan, Mao Guo, Yongliang Liu, Shiqi Li, Huimin Fan, Yanchun Zhao, Gang Zhong, Songxiong Liu, Cun Luo, Xubiao Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle Nanchang Hangkong University Nanchang330063 China Jiangxi Academy of Eco-Environmental Sciences and Planning Nanchang330006 China Institute of Eco-Environmental and Soil Sciences Guangdong Academy of Sciences Guangzhou510650 China Key Laboratory of Soil Environment and Pollution Remediation Institute of Soil Science Chinese Academy of Sciences Nanjing210008 China National-Local Joint Engineering Research Center of Heavy Metal Pollutants Control and Resource Utilization

Individual application of sulfide modification and electromagnetic field (EMF) can enhance the reaction efficiency of nanoscale zero-valent iron (nZVI), yet the potential of both in combination is not clear. This work found that the reactivity of nZVI towards decabromodiphenyl ether was significantly enhanced by the combined effect of sulfide modification and EMF, and the specific reaction rate constant increased by a factor of 7 to 10. A series of characterization results revealed that the sulfidation level not only affects the inherent reactivity but also the magnetic-induced heating (MIH) capacity and magnetic-induced corrosion (MIC) of nZVI, which collectively influence the degradation efficiency of nZVI under EMF. Sulfidation generally diminished the MIH effect. The low degree of sulfidation (S/Fe = 0.1) slightly reduced the MIC effect while the high degree of sulfidation (S/Fe = 0.4) led to significantly enhanced MIC effect. For S/Fe = 0.1 and 0.4, the overall enhancement in the reactivity resulting from EMF was alternately dominated by the contributions of MIH and MIC. This work provides valuable insights into the magnitude of MIH and MIC in relation to the sulfidation level of nZVI, which is needed for further exploration and optimization of this combined technology. © 2023, The Authors. All rights reserved.

关键词： Electromagnetic fields

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