Bin Wang, Yue Xuan, Shuai Meng, Wenjie Fan, Yanjie Liang, Yue Peng, Qiaowan Chang, Tao Luan, Dong Wang, Junhua Li
Enriching oxygen species in perovskite catalysts provides more active sites for the catalytic oxidation of air pollutants, but its further application in environmental chemical engineering is still constrained by the inherent lack of oxygen species reactivity and the difficulty of replenishing depleted oxygen species. Herein, we present a scalable one-pot strategy for the in situ fabrication of a homogeneously distributed heterostructure, which brings La2CuO4 perovskite a 58-fold activity enhancement and robust antisintering/water/coke in toluene oxidation, higher than currently reported perovskite catalysts. Superior to the single “oxygen enrichment” effect of conventional surface-aggregated heterostructures, the homogeneously distributed heterostructures induce the reactivity enhancement of adsorbed oxygen and the backfilling/replenishment of depleted lattice oxygen, which break through the rate-determining steps of the low-temperature Langmuir–Hinshelwood and the high-temperature Mars–van Krevelen mechanisms, respectively. The scalability has been demonstrated in broader perovskite systems and for oxygen evolution reaction, offering a more dependable oxygen supply for environmental catalysis.
{"title":"Homogeneously Distributed Heterostructure Energizes and Replenishes Oxygen Species for Boosting Toluene Oxidation on Perovskite Oxide Catalysts","authors":"Bin Wang, Yue Xuan, Shuai Meng, Wenjie Fan, Yanjie Liang, Yue Peng, Qiaowan Chang, Tao Luan, Dong Wang, Junhua Li","doi":"10.1021/acs.est.4c09900","DOIUrl":"https://doi.org/10.1021/acs.est.4c09900","url":null,"abstract":"Enriching oxygen species in perovskite catalysts provides more active sites for the catalytic oxidation of air pollutants, but its further application in environmental chemical engineering is still constrained by the inherent lack of oxygen species reactivity and the difficulty of replenishing depleted oxygen species. Herein, we present a scalable one-pot strategy for the in situ fabrication of a homogeneously distributed heterostructure, which brings La<sub>2</sub>CuO<sub>4</sub> perovskite a 58-fold activity enhancement and robust antisintering/water/coke in toluene oxidation, higher than currently reported perovskite catalysts. Superior to the single “oxygen enrichment” effect of conventional surface-aggregated heterostructures, the homogeneously distributed heterostructures induce the reactivity enhancement of adsorbed oxygen and the backfilling/replenishment of depleted lattice oxygen, which break through the rate-determining steps of the low-temperature Langmuir–Hinshelwood and the high-temperature Mars–van Krevelen mechanisms, respectively. The scalability has been demonstrated in broader perovskite systems and for oxygen evolution reaction, offering a more dependable oxygen supply for environmental catalysis.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"23 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569921","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kang Liu, Xiaohong Zhu, Yuying Zhang, Mengmeng Wang, Roya Maboudian, Daniel S. Alessi, Daniel C.W. Tsang
The temperature for complete disintegration of spent lithium-ion battery (LIB) cathode materials is typically in a range of 750–1400 °C, resulting in intensive energy consumption and high carbon emissions. Here, we promote the bond activation of oxygen in LiNi0.5Co0.2Mn0.3O2 and carbon in graphite electrodes, achieving rapid gasification and thermal decomposition of active crystals at lower temperatures in the absence of other activating agents. The activation of C and O bond leads to the storage of internal energy and the transition of the crystalline phase (single crystal to polycrystal) of the active crystals. Density functional theory modeling confirms that the CO adsorption energy is significantly higher with Ca–Oa (−3.35 eV, C and O activation) than with no activation (−1.66 eV). The differential charge results show that the bond activation model has the highest charge accumulation and consumption, improving the electron transfer. The Bader charge transfer between Ca–Oa and CO is also the largest, with a value of 0.433 |e|. Therefore, synchronous activation of C and O bonds can reduce the decomposition temperature of active crystals by 200 °C and allows a low-temperature pyrolysis recycling of retired LIB cathode materials. Our research provides a potential strategy for low-carbon recycling of retired LIBs worldwide.
{"title":"Activating Carbon and Oxygen Bonds for Low-Temperature Thermal Decomposition of Spent Lithium-Ion Battery Cathode Materials","authors":"Kang Liu, Xiaohong Zhu, Yuying Zhang, Mengmeng Wang, Roya Maboudian, Daniel S. Alessi, Daniel C.W. Tsang","doi":"10.1021/acs.est.4c12200","DOIUrl":"https://doi.org/10.1021/acs.est.4c12200","url":null,"abstract":"The temperature for complete disintegration of spent lithium-ion battery (LIB) cathode materials is typically in a range of 750–1400 °C, resulting in intensive energy consumption and high carbon emissions. Here, we promote the bond activation of oxygen in LiNi<sub>0.5</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>O<sub>2</sub> and carbon in graphite electrodes, achieving rapid gasification and thermal decomposition of active crystals at lower temperatures in the absence of other activating agents. The activation of C and O bond leads to the storage of internal energy and the transition of the crystalline phase (single crystal to polycrystal) of the active crystals. Density functional theory modeling confirms that the CO adsorption energy is significantly higher with C<sub><i>a</i></sub>–O<sub><i>a</i></sub> (−3.35 eV, C and O activation) than with no activation (−1.66 eV). The differential charge results show that the bond activation model has the highest charge accumulation and consumption, improving the electron transfer. The Bader charge transfer between C<sub><i>a</i></sub>–O<sub><i>a</i></sub> and CO is also the largest, with a value of 0.433 |e|. Therefore, synchronous activation of C and O bonds can reduce the decomposition temperature of active crystals by 200 °C and allows a low-temperature pyrolysis recycling of retired LIB cathode materials. Our research provides a potential strategy for low-carbon recycling of retired LIBs worldwide.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"93 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560768","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Gaojie Chen, Xiaolong Fan, Shaocai Yu, Yee Jun Tham, Ziyi Lin, Xiaoting Ji, Lingling Xu, Jinsheng Chen
Chlorine (Cl) radicals can profoundly affect the atmospheric oxidation capacity and the fates of pollutants. Hypochlorous acid (HOCl) is a potentially crucial Cl precursor, yet the understanding of its formation mechanisms and atmospheric impacts is still limited. Here, we observed high concentrations of HOCl in a coastal city of Southeast China during the autumn of 2022, with an average daytime peak of 181 ppt. Machine learning analysis identified Cl2, O3, nitrate, temperature, and iron as the primary factors affecting HOCl distribution. Beyond Cl2 photolysis, both nitrate photolysis and aerosol iron photochemistry also contributed to Cl radical production, which drove daytime HOCl production through reactions involving ClO and HO2 radicals in the presence of O3. Both OH and Cl radicals released via HOCl photolysis increased the levels of ROx radicals by ∼10%, thereby enhancing the daytime O3 generation and atmospheric oxidation capacity. Our findings emphasize the significant role of HOCl in atmospheric chemistry and suggest that controlling O3 levels could alleviate Cl radical production and its adverse impacts on air quality.
{"title":"HOCl Formation Driven by Photochemical Processes Enhanced Atmospheric Oxidation Capacity in a Coastal Atmosphere","authors":"Gaojie Chen, Xiaolong Fan, Shaocai Yu, Yee Jun Tham, Ziyi Lin, Xiaoting Ji, Lingling Xu, Jinsheng Chen","doi":"10.1021/acs.est.5c01363","DOIUrl":"https://doi.org/10.1021/acs.est.5c01363","url":null,"abstract":"Chlorine (Cl) radicals can profoundly affect the atmospheric oxidation capacity and the fates of pollutants. Hypochlorous acid (HOCl) is a potentially crucial Cl precursor, yet the understanding of its formation mechanisms and atmospheric impacts is still limited. Here, we observed high concentrations of HOCl in a coastal city of Southeast China during the autumn of 2022, with an average daytime peak of 181 ppt. Machine learning analysis identified Cl<sub>2</sub>, O<sub>3</sub>, nitrate, temperature, and iron as the primary factors affecting HOCl distribution. Beyond Cl<sub>2</sub> photolysis, both nitrate photolysis and aerosol iron photochemistry also contributed to Cl radical production, which drove daytime HOCl production through reactions involving ClO and HO<sub>2</sub> radicals in the presence of O<sub>3</sub>. Both OH and Cl radicals released via HOCl photolysis increased the levels of RO<i><sub><i>x</i></sub></i> radicals by ∼10%, thereby enhancing the daytime O<sub>3</sub> generation and atmospheric oxidation capacity. Our findings emphasize the significant role of HOCl in atmospheric chemistry and suggest that controlling O<sub>3</sub> levels could alleviate Cl radical production and its adverse impacts on air quality.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"45 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560774","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Masato Ooka, Jinghua Zhao, Li Zhang, Ruili Huang, Srilatha Sakamuru, Charlotte TeKrony, Jui-Hua Hsieh, Bradley J. Collins, June K. Dunnick, Darlene Dixon, Menghang Xia
Superfund sites are where soil, air, and water are polluted with hazardous materials. Individuals residing and working in these areas are often exposed to metals and other hazardous materials, leading to many adverse health outcomes, including cancer. While individuals are often exposed to multiple chemicals simultaneously, the combined effect of such exposures remains largely unexplored. Here, we investigated the toxicity of metal mixtures in five categories of in vitro assays measuring cytotoxicity, oxidative stress, genotoxicity, cytokine release, and angiogenesis. After testing these mixtures in primary cells and cell lines, we discovered that the nickel/arsenic/cadmium and beryllium/arsenic/cadmium combinations exhibited higher cytotoxicity than their individual compounds, suggesting that the mixtures amplified the cytotoxic effect. To investigate the mechanism underlying their toxicity, we evaluated metal-induced oxidative stress, as oxidative stress is a common factor in most metal-related toxicities. Our results showed that cadmium-induced oxidative stress was increased in mixtures. Some mixtures that induced oxidative stress further increased DNA damage, inhibited DNA synthesis, and activated p53. In addition, some mixtures significantly increased interleukin-8 secretion and angiogenesis more than their component compounds. Our findings offer important insights into metal-related toxicity at Superfund sites.
超级基金场所是土壤、空气和水受到有害物质污染的地方。在这些地区居住和工作的人经常会接触到金属和其他有害物质，从而导致许多不良的健康后果，包括癌症。虽然人们经常会同时接触多种化学物质，但这些接触的综合效应在很大程度上仍未得到研究。在这里，我们通过五类体外实验研究了金属混合物的毒性，分别测量细胞毒性、氧化应激、基因毒性、细胞因子释放和血管生成。在原代细胞和细胞系中对这些混合物进行测试后，我们发现镍/砷/镉和铍/砷/镉混合物的细胞毒性高于其单个化合物，这表明混合物放大了细胞毒性效应。为了研究其毒性的机制，我们评估了金属诱导的氧化应激，因为氧化应激是大多数金属相关毒性的共同因素。结果表明，镉诱导的氧化应激在混合物中有所增加。一些诱导氧化应激的混合物进一步加剧了 DNA 损伤，抑制了 DNA 合成，并激活了 p53。此外，一些混合物比其成分化合物更能显著增加白细胞介素-8的分泌和血管生成。我们的研究结果为了解超级基金场地中与金属有关的毒性提供了重要启示。
{"title":"Profiling of Environmental Mixtures Containing Metals for Their Toxicity Pathways and Mechanism of Action","authors":"Masato Ooka, Jinghua Zhao, Li Zhang, Ruili Huang, Srilatha Sakamuru, Charlotte TeKrony, Jui-Hua Hsieh, Bradley J. Collins, June K. Dunnick, Darlene Dixon, Menghang Xia","doi":"10.1021/acs.est.4c07995","DOIUrl":"https://doi.org/10.1021/acs.est.4c07995","url":null,"abstract":"Superfund sites are where soil, air, and water are polluted with hazardous materials. Individuals residing and working in these areas are often exposed to metals and other hazardous materials, leading to many adverse health outcomes, including cancer. While individuals are often exposed to multiple chemicals simultaneously, the combined effect of such exposures remains largely unexplored. Here, we investigated the toxicity of metal mixtures in five categories of <i>in vitro</i> assays measuring cytotoxicity, oxidative stress, genotoxicity, cytokine release, and angiogenesis. After testing these mixtures in primary cells and cell lines, we discovered that the nickel/arsenic/cadmium and beryllium/arsenic/cadmium combinations exhibited higher cytotoxicity than their individual compounds, suggesting that the mixtures amplified the cytotoxic effect. To investigate the mechanism underlying their toxicity, we evaluated metal-induced oxidative stress, as oxidative stress is a common factor in most metal-related toxicities. Our results showed that cadmium-induced oxidative stress was increased in mixtures. Some mixtures that induced oxidative stress further increased DNA damage, inhibited DNA synthesis, and activated p53. In addition, some mixtures significantly increased interleukin-8 secretion and angiogenesis more than their component compounds. Our findings offer important insights into metal-related toxicity at Superfund sites.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"11 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560769","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhiyu Pan, Xunheng Jiang, Xia Feng, Yi Liu, Wenhua Dong, Yue Chen, Can Li, Bijun Yang, Jie Hou, Jianying Zhang, Lizhong Zhu, Daohui Lin, Jiang Xu
Nonradical Fenton-like catalysis offers an opportunity to degrade extracellular antibiotic resistance genes (eARGs). However, high-loading single-atom catalysts (SACs) with controllable configurations are urgently required to selectively generate high-yield nonradicals. Herein, we constructed high-loading Fe SACs (5.4–34.2 wt %) with uniform Fe–N4 sites via an optimized coordination balance of supermolecular assembly for peroxymonosulfate activation. The selectivity of singlet oxygen (1O2) generation and its contribution to eARGs degradation were both >98%. This targeting strategy of oxidizing guanines with low ionization potentials by 1O2 allowed 7 log eARGs degradation within 10 min and eliminated their transformation within 2 min, outperforming most reported advanced oxidation processes. Relevant interactions between 1O2 and guanines were revealed at a single-molecule resolution. The high-loading Fe SACs exhibited excellent universality and stability for different eARGs and water matrices. These findings provide a promising route for constructing high-loading SACs for efficient and selective Fenton-like water treatment.
{"title":"Controllable Supply–Demand Effect during Superior Fe Single-Atom Catalyst Synthesis for Targeted Guanine Oxidation of Antibiotic Resistance Genes","authors":"Zhiyu Pan, Xunheng Jiang, Xia Feng, Yi Liu, Wenhua Dong, Yue Chen, Can Li, Bijun Yang, Jie Hou, Jianying Zhang, Lizhong Zhu, Daohui Lin, Jiang Xu","doi":"10.1021/acs.est.4c13667","DOIUrl":"https://doi.org/10.1021/acs.est.4c13667","url":null,"abstract":"Nonradical Fenton-like catalysis offers an opportunity to degrade extracellular antibiotic resistance genes (eARGs). However, high-loading single-atom catalysts (SACs) with controllable configurations are urgently required to selectively generate high-yield nonradicals. Herein, we constructed high-loading Fe SACs (5.4–34.2 wt %) with uniform Fe–N<sub>4</sub> sites via an optimized coordination balance of supermolecular assembly for peroxymonosulfate activation. The selectivity of singlet oxygen (<sup>1</sup>O<sub>2</sub>) generation and its contribution to eARGs degradation were both >98%. This targeting strategy of oxidizing guanines with low ionization potentials by <sup>1</sup>O<sub>2</sub> allowed 7 log eARGs degradation within 10 min and eliminated their transformation within 2 min, outperforming most reported advanced oxidation processes. Relevant interactions between <sup>1</sup>O<sub>2</sub> and guanines were revealed at a single-molecule resolution. The high-loading Fe SACs exhibited excellent universality and stability for different eARGs and water matrices. These findings provide a promising route for constructing high-loading SACs for efficient and selective Fenton-like water treatment.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"91 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560771","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ultraviolet light-induced homolysis of hydrogen peroxide (UV/H2O2) can generate powerful hydroxyl radicals (•OH) for sustainable water purification. However, the efficiency of the conventional bulk-phase UV/H2O2 system is limited by the low yield and utilization of •OH, in turn necessitating high UV energy input and long purification period. In this study, we present an innovative UV/H2O2 microdroplet system for enhanced pollutant degradation. The degradation of pollutants in sprayed microdroplets was accelerated by 8.5–63.3-fold compared to those in bulk water, demonstrating universal effectiveness across a range of pollutant types and diverse aqueous matrices. This enhancement stems from elevated •OH production at the air–water interface due to the enhanced UV absorbance of H2O2. The production of •OH in the microdroplet system was 45-fold higher than that in bulk water, facilitating rapid •OH-mediated pollutant degradation. Moreover, pollutants accumulate at the air–water interface, where •OH is concentrated, leading to higher utilization of •OH for mediating pollutant degradation before quenching. Our findings provide a solution to overcome the bottlenecks in •OH production and utilization, offering insights for improving the efficiency of UV/H2O2 water treatment systems.
{"title":"Accelerated Pollutant Degradation by UV/H2O2 at the Air–Water Interface of Microdroplets","authors":"Xiaochen Liu, Yishuai Pan, Yu Yao, Shuxuan Chen, Baoliang Chen, Chiheng Chu","doi":"10.1021/acs.est.4c14592","DOIUrl":"https://doi.org/10.1021/acs.est.4c14592","url":null,"abstract":"Ultraviolet light-induced homolysis of hydrogen peroxide (UV/H<sub>2</sub>O<sub>2</sub>) can generate powerful hydroxyl radicals (<sup>•</sup>OH) for sustainable water purification. However, the efficiency of the conventional bulk-phase UV/H<sub>2</sub>O<sub>2</sub> system is limited by the low yield and utilization of <sup>•</sup>OH, in turn necessitating high UV energy input and long purification period. In this study, we present an innovative UV/H<sub>2</sub>O<sub>2</sub> microdroplet system for enhanced pollutant degradation. The degradation of pollutants in sprayed microdroplets was accelerated by 8.5–63.3-fold compared to those in bulk water, demonstrating universal effectiveness across a range of pollutant types and diverse aqueous matrices. This enhancement stems from elevated <sup>•</sup>OH production at the air–water interface due to the enhanced UV absorbance of H<sub>2</sub>O<sub>2</sub>. The production of <sup>•</sup>OH in the microdroplet system was 45-fold higher than that in bulk water, facilitating rapid <sup>•</sup>OH-mediated pollutant degradation. Moreover, pollutants accumulate at the air–water interface, where <sup>•</sup>OH is concentrated, leading to higher utilization of <sup>•</sup>OH for mediating pollutant degradation before quenching. Our findings provide a solution to overcome the bottlenecks in <sup>•</sup>OH production and utilization, offering insights for improving the efficiency of UV/H<sub>2</sub>O<sub>2</sub> water treatment systems.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"191 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560772","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nondispersive infrared (NDIR) sensors offer high sensitivity, selectivity, and low operational costs, making them particularly well-suited for environmental gas monitoring, where accurate detection of gases such as CH4 and CO2 is essential. However, these sensors are highly sensitive to environmental conditions, including temperature and humidity, which can significantly affect detection accuracy. This study characterizes the effects of these conditions and applies machine learning models to correct signal biases caused by multiple environmental factors. Experiments simulating natural environmental conditions for CH4 monitoring were conducted in the laboratory across a temperature range of 10–40 °C, relative humidity levels of 10–70%, and CO2 concentrations ranging from 0 to 1000 ppm, revealing significant signal variability under these conditions. The simulations and their results were comprehensively validated at the Ito Natural Analogue Site (INAS), a real-world field-testing location dedicated to investigating environmental impacts. Using machine learning regression algorithms for comprehensive compensation of environmental influences, we successfully mitigated signal biases caused by environmental factors. This offers a cost-effective solution for improving detection accuracy and reliability while reducing system complexity and operational costs.
{"title":"Environmental Effects on NDIR-Based CH4 Monitoring: Characterization and Correction","authors":"Wei Dong, Kyuro Sasaki, Hemeng Zhang, Yongjun Wang, Xiaoming Zhang, Yuichi Sugai","doi":"10.1021/acs.est.4c11110","DOIUrl":"https://doi.org/10.1021/acs.est.4c11110","url":null,"abstract":"Nondispersive infrared (NDIR) sensors offer high sensitivity, selectivity, and low operational costs, making them particularly well-suited for environmental gas monitoring, where accurate detection of gases such as CH<sub>4</sub> and CO<sub>2</sub> is essential. However, these sensors are highly sensitive to environmental conditions, including temperature and humidity, which can significantly affect detection accuracy. This study characterizes the effects of these conditions and applies machine learning models to correct signal biases caused by multiple environmental factors. Experiments simulating natural environmental conditions for CH<sub>4</sub> monitoring were conducted in the laboratory across a temperature range of 10–40 °C, relative humidity levels of 10–70%, and CO<sub>2</sub> concentrations ranging from 0 to 1000 ppm, revealing significant signal variability under these conditions. The simulations and their results were comprehensively validated at the Ito Natural Analogue Site (INAS), a real-world field-testing location dedicated to investigating environmental impacts. Using machine learning regression algorithms for comprehensive compensation of environmental influences, we successfully mitigated signal biases caused by environmental factors. This offers a cost-effective solution for improving detection accuracy and reliability while reducing system complexity and operational costs.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"10 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560778","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Provincial inherent heterogeneity in resource endowment, steel demand, and managerial guidance poses not only challenges but also chances to the decarbonization of China’s iron and steel industry (ISI). Previous studies have primarily concentrated on the technological dimension at the national level or plant level but have neglected potential regional synergies. This study proposed a framework encompassing macroeconomic models and multi-objective algorithms to optimize interprovincial allocation of scrap resources for coordinating the steelmaking process transition, aiming to minimize total carbon emissions from ISI. Results indicate that optimizing scrap allocation can reduce carbon emissions by 173.97–215.66 million tons, achieving a 99% reduction by 2060 compared to 2020 levels. Under the coordination strategy, 19 out of 28 provinces can achieve carbon neutrality and realize more than 90% pollutant reduction in the ISI. Notably, provinces such as Hebei, Inner Mongolia, Shanxi, Heilongjiang, and Liaoning still need to import more scrap resources and implement innovative low-carbon technologies. Finally, we propose interprovincial coordinated transition strategies, including regional integration management, national data platform, and preferential economic instrument. This work guides national and provincial administrations to formulate differentiated low-carbon transition targets and collaborative actions in ISI, which can be also applied to other substantially heterogeneous industries to achieve carbon neutrality.
{"title":"Coordinating Interprovincial Scrap Supply for Technology Transition to Minimize Carbon Emissions of China’s Iron and Steel Industry","authors":"Zewei Lin, Chen Cai, Yumeng Zhang, Xiaomin Zhu, Fangyin Peng, Ru Guo, Kaiming Peng, Xiangfeng Huang, Yongjie Zhang, Guojun Chen, Jia Liu","doi":"10.1021/acs.est.4c12188","DOIUrl":"https://doi.org/10.1021/acs.est.4c12188","url":null,"abstract":"Provincial inherent heterogeneity in resource endowment, steel demand, and managerial guidance poses not only challenges but also chances to the decarbonization of China’s iron and steel industry (ISI). Previous studies have primarily concentrated on the technological dimension at the national level or plant level but have neglected potential regional synergies. This study proposed a framework encompassing macroeconomic models and multi-objective algorithms to optimize interprovincial allocation of scrap resources for coordinating the steelmaking process transition, aiming to minimize total carbon emissions from ISI. Results indicate that optimizing scrap allocation can reduce carbon emissions by 173.97–215.66 million tons, achieving a 99% reduction by 2060 compared to 2020 levels. Under the coordination strategy, 19 out of 28 provinces can achieve carbon neutrality and realize more than 90% pollutant reduction in the ISI. Notably, provinces such as Hebei, Inner Mongolia, Shanxi, Heilongjiang, and Liaoning still need to import more scrap resources and implement innovative low-carbon technologies. Finally, we propose interprovincial coordinated transition strategies, including regional integration management, national data platform, and preferential economic instrument. This work guides national and provincial administrations to formulate differentiated low-carbon transition targets and collaborative actions in ISI, which can be also applied to other substantially heterogeneous industries to achieve carbon neutrality.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"23 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546055","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yongjin Xiang, Jingtao Hou, Lu Ren, Juan Xiong, Biao Wan, Mingxia Wang, Wenfeng Tan, Andreas Kappler
The reduction of As(V) to As(III) has been proposed as an undesirable process, increasing the mobility and toxicity of arsenic. Although most studies revealed that As(V) reduction occurs in the aqueous phase, it remains unclear whether abiotic As(V) reduction driven by minerals in drought environments also exists. In this study, we examined the transformation of As(V) to As(III) mediated by ferrihydrite during drying processes using high-resolution X-ray photoelectron spectroscopy (XPS) and X-ray absorption near edge structure (XANES) spectroscopy analyses. The results revealed that nearly 40.8% of ferrihydrite-sorbed As(V) was transformed to As(III) after placing the As(V)-adsorbed ferrihydrite solids in a drought-tolerant environment for 7 days. As(V) reduction occurred under both oxic and anoxic conditions, with the reduction rate being higher in an anoxic atmosphere than in oxygen and air. Chemical analysis revealed the presence of structural Fe(II) in ferrihydrite, which was attributed to the abundance of oxygen vacancy clusters, as evidenced by positron annihilation lifetime (PAL) analysis. Fe L-edge XANES analysis and DFT calculations demonstrated that structural Fe(II) in dried ferrihydrite played a vital role in As(V) reduction, inducing electron transfer from Fe to As atoms. The findings of this study highlight a potentially important but long-overlooked As(V) reduction pathway at mineral surfaces under drought conditions in dried soils.
{"title":"Spontaneous Abiotic Reduction of Arsenate to Arsenite Mediated by Structural Fe(II) Resulting from Abundant Oxygen Vacancy Clusters in Poorly Crystalline Ferrihydrite in Drought Environments","authors":"Yongjin Xiang, Jingtao Hou, Lu Ren, Juan Xiong, Biao Wan, Mingxia Wang, Wenfeng Tan, Andreas Kappler","doi":"10.1021/acs.est.4c10674","DOIUrl":"https://doi.org/10.1021/acs.est.4c10674","url":null,"abstract":"The reduction of As(V) to As(III) has been proposed as an undesirable process, increasing the mobility and toxicity of arsenic. Although most studies revealed that As(V) reduction occurs in the aqueous phase, it remains unclear whether abiotic As(V) reduction driven by minerals in drought environments also exists. In this study, we examined the transformation of As(V) to As(III) mediated by ferrihydrite during drying processes using high-resolution X-ray photoelectron spectroscopy (XPS) and X-ray absorption near edge structure (XANES) spectroscopy analyses. The results revealed that nearly 40.8% of ferrihydrite-sorbed As(V) was transformed to As(III) after placing the As(V)-adsorbed ferrihydrite solids in a drought-tolerant environment for 7 days. As(V) reduction occurred under both oxic and anoxic conditions, with the reduction rate being higher in an anoxic atmosphere than in oxygen and air. Chemical analysis revealed the presence of structural Fe(II) in ferrihydrite, which was attributed to the abundance of oxygen vacancy clusters, as evidenced by positron annihilation lifetime (PAL) analysis. Fe L-edge XANES analysis and DFT calculations demonstrated that structural Fe(II) in dried ferrihydrite played a vital role in As(V) reduction, inducing electron transfer from Fe to As atoms. The findings of this study highlight a potentially important but long-overlooked As(V) reduction pathway at mineral surfaces under drought conditions in dried soils.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"36 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560777","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Increasing microplastic (MP) inputs in agricultural soils have gained global attention for their ecological effects, especially on soil organic carbon (SOC) and nutrient turnover. However, the microbial mechanism underlying MP-induced SOC and nutrient dynamics remains poorly understood. Here, we investigated the impacts of two common MPs (polyethylene and polyvinyl chloride) on microbial hierarchical groups (bacteria, fungi, and protists) and the cascading effects on dissolved organic carbon (DOC) and nutrient dynamics in two typical agricultural soils (Mollisol and Ultisol). Our results showed that MP inputs consistently reduced NO3––N concentration but increased the content of DOC and specific dissolved organic matter (DOM) components. Despite divergent responses of microbial hierarchical groups to MPs, MP inputs consistently strengthened the connectivity and cross-trophic associations of microbial multitrophic networks. Protistan nodes belonging to Cercozoa, Ciliophora, and Chlorophyta played essential roles in maintaining network connectivity in MP-treated soils. The enhanced network connectivity and cross-trophic associations primarily explained variations in soil DOC and nutrient turnover. These findings collectively indicate that MP inputs trigger DOC and nutrient turnover by enhancing the potential multitrophic interactions and species connectivity within soil micro-food webs. Our study provides novel insights into the ecological consequences of MP pollution on microbial hierarchical interactions and microbially mediated biogeochemical cycling.
{"title":"Microplastics Trigger Soil Dissolved Organic Carbon and Nutrient Turnover by Strengthening Microbial Network Connectivity and Cross-Trophic Interactions","authors":"Shenghan Gao, Yunbo Fu, Xinyi Peng, Silin Ma, Yu-Rong Liu, Wenli Chen, Qiaoyun Huang, Xiuli Hao","doi":"10.1021/acs.est.4c12546","DOIUrl":"https://doi.org/10.1021/acs.est.4c12546","url":null,"abstract":"Increasing microplastic (MP) inputs in agricultural soils have gained global attention for their ecological effects, especially on soil organic carbon (SOC) and nutrient turnover. However, the microbial mechanism underlying MP-induced SOC and nutrient dynamics remains poorly understood. Here, we investigated the impacts of two common MPs (polyethylene and polyvinyl chloride) on microbial hierarchical groups (bacteria, fungi, and protists) and the cascading effects on dissolved organic carbon (DOC) and nutrient dynamics in two typical agricultural soils (Mollisol and Ultisol). Our results showed that MP inputs consistently reduced NO<sub>3</sub><sup>–</sup>–N concentration but increased the content of DOC and specific dissolved organic matter (DOM) components. Despite divergent responses of microbial hierarchical groups to MPs, MP inputs consistently strengthened the connectivity and cross-trophic associations of microbial multitrophic networks. Protistan nodes belonging to Cercozoa, Ciliophora, and Chlorophyta played essential roles in maintaining network connectivity in MP-treated soils. The enhanced network connectivity and cross-trophic associations primarily explained variations in soil DOC and nutrient turnover. These findings collectively indicate that MP inputs trigger DOC and nutrient turnover by enhancing the potential multitrophic interactions and species connectivity within soil micro-food webs. Our study provides novel insights into the ecological consequences of MP pollution on microbial hierarchical interactions and microbially mediated biogeochemical cycling.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"32 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546058","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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