Pub Date : 2026-02-04DOI: 10.1016/j.seppur.2026.137161
Dong A. Kang, Blake Trusty, Shailesh Dangwal, Benjamin T. Manard, Jordan S. Stanberry, Mariappan Parans Paranthaman, Ramesh R. Bhave, Syed Z. Islam
Rare earth elements (REEs) are essential for advanced technologies and yet face significant supply chain risks due to their concentrated global production and limited domestic availability. Addressing this challenge requires efficient processes capable of upgrading low-grade secondary resources such as mine tailings. In this study, we developed a novel separation flowsheet that integrates sequential leaching and 2-stage solvent extraction (SX) processes to recover high-purity heavy REEs (HREEs) and light REEs (LREEs) from a simulated mine-tailing concentrate containing 2.4 wt% total REEs (TREEs; 0.6 wt% LREEs and 1.8 wt% HREEs). Sequential leaching with controlled pH adjustment selectively precipitated REEs while retaining the large amount of impurities in the solution, producing an REE-enriched leachate by following leaching processes with roughly twice the REE concentration and half the impurity concentration compared to that of single-step leaching. The optimized SX flowsheet employed Cyanex 572 to extract HREEs and Fe over LREEs, followed by Fe removal using tributyl phosphate (TBP), while the raffinate stream was processed by SX with di(2-ethylhexyl)phosphoric acid (D2EHPA) to recover LREEs under optimized conditions balancing both extraction efficiency and purity. Although increased extractant availability in the organic phase improved LREE recovery, it also increased co-extraction of Ca, underscoring trade-offs in process optimization. Both HREE- and LREE-rich solutions were subsequently precipitated into solid products via oxalate precipitation, resulting in high-purity REE solids containing ~92.0 wt% HREEs (~ 95.7 wt% TREEs) and ~ 92.8 wt% LREEs (~ 94.0 wt% TREEs). This proof-of-concept study using simulated mine tailings demonstrates a promising approach for upgrading low-grade REE resources, while highlighting the need for future validation with real materials.
{"title":"Process design for recovering rare-earth elements from mine tailings with low rare-earth concentrations via sequential leaching and solvent extraction","authors":"Dong A. Kang, Blake Trusty, Shailesh Dangwal, Benjamin T. Manard, Jordan S. Stanberry, Mariappan Parans Paranthaman, Ramesh R. Bhave, Syed Z. Islam","doi":"10.1016/j.seppur.2026.137161","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.137161","url":null,"abstract":"Rare earth elements (REEs) are essential for advanced technologies and yet face significant supply chain risks due to their concentrated global production and limited domestic availability. Addressing this challenge requires efficient processes capable of upgrading low-grade secondary resources such as mine tailings. In this study, we developed a novel separation flowsheet that integrates sequential leaching and 2-stage solvent extraction (SX) processes to recover high-purity heavy REEs (HREEs) and light REEs (LREEs) from a simulated mine-tailing concentrate containing 2.4 wt% total REEs (TREEs; 0.6 wt% LREEs and 1.8 wt% HREEs). Sequential leaching with controlled pH adjustment selectively precipitated REEs while retaining the large amount of impurities in the solution, producing an REE-enriched leachate by following leaching processes with roughly twice the REE concentration and half the impurity concentration compared to that of single-step leaching. The optimized SX flowsheet employed Cyanex 572 to extract HREEs and Fe over LREEs, followed by Fe removal using tributyl phosphate (TBP), while the raffinate stream was processed by SX with di(2-ethylhexyl)phosphoric acid (D2EHPA) to recover LREEs under optimized conditions balancing both extraction efficiency and purity. Although increased extractant availability in the organic phase improved LREE recovery, it also increased co-extraction of Ca, underscoring trade-offs in process optimization. Both HREE- and LREE-rich solutions were subsequently precipitated into solid products via oxalate precipitation, resulting in high-purity REE solids containing ~92.0 wt% HREEs (~ 95.7 wt% TREEs) and ~ 92.8 wt% LREEs (~ 94.0 wt% TREEs). This proof-of-concept study using simulated mine tailings demonstrates a promising approach for upgrading low-grade REE resources, while highlighting the need for future validation with real materials.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"15 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116138","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Solar-driven interfacial evaporators (SDIEs) have advanced sustainable desalination by enabling freshwater production and salt harvesting from brines. Here, electrospun cellulose acetate (CA) films with aligned nanoporous fibers are rolled into a 3D cylinder and partially coated with a carbon black/poly(vinyl alcohol) (CB/PVA) photothermal layer to create an environmentally-friendly SDIE for concurrent desalination and salt recovery. The evaporator achieves a high evaporation rate of 4.44 kg m−2 h−1 under 1 sun, corresponding to a photothermal conversion efficiency of 107.3% based on equivalent evaporation enthalpy. This performance is ascribed to reduced vaporization enthalpy from material-water interactions and nanoporous structures, along with cold evaporation-induced environmental energy harvesting. Under 1 sun, the SDIE stably treats brines of 3.5–20 wt% salinity with edge-preferential salt crystallization due to its fibrous microporous architecture. This feature allows gravity-assisted salt collection and durable function in 10 wt% NaCl for 10 days, maintaining average steam generation and salt harvesting rates of 4.71 kg m−2 h−1 and 3.21 kg m−2 day−1, respectively. Condensed waters from 3.5 wt% NaCl and simulated seawater exhibit high purity with significantly lower conductivities. The outdoor experiment also reveals the stable performance of the SDIE under actual conditions. Computational fluid dynamics (CFD) simulation further validates edge-preferential salt aggregation. This innovative device offers a promising route for simultaneous freshwater and salt collection from brines.
太阳能驱动的界面蒸发器(SDIEs)通过实现淡水生产和从盐水中收集盐,推动了可持续的海水淡化。在这里,电纺醋酸纤维素(CA)薄膜与排列整齐的纳米多孔纤维被卷成一个3D圆柱体,并部分涂上炭黑/聚乙烯醇(CB/PVA)光热层,以创建一个环保的SDIE,用于同时脱盐和盐回收。蒸发器在1个太阳下的蒸发速率高达4.44 kg m−2 h−1,根据等效蒸发焓计算,光热转换效率为107.3%。这种性能归因于材料-水相互作用和纳米孔结构的蒸发焓降低,以及冷蒸发引起的环境能量收集。在1个太阳下,由于其纤维微孔结构,SDIE稳定地处理盐度为3.5 - 20%的盐水,并具有边缘优先的盐结晶。该功能允许重力辅助盐收集和在10 wt% NaCl中持续10天,保持平均蒸汽产生和盐收集率分别为4.71 kg m−2 h−1和3.21 kg m−2 day−1。3.5 wt% NaCl和模拟海水的凝结水纯度高,电导率明显降低。室外实验也显示了SDIE在实际条件下的稳定性能。计算流体动力学(CFD)模拟进一步验证了边缘优先的盐聚集。这种创新的设备为同时从盐水中收集淡水和盐提供了一条有前途的途径。
{"title":"Nanoporous fibrous 3D solar evaporator for efficient freshwater generation and salt recovery","authors":"Mojtaba Ebrahimian Mashhadi, Md. Mehadi Hassan, Ningxin Chen, Ruijie Yang, Qingye Lu","doi":"10.1016/j.seppur.2026.137162","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.137162","url":null,"abstract":"Solar-driven interfacial evaporators (SDIEs) have advanced sustainable desalination by enabling freshwater production and salt harvesting from brines. Here, electrospun cellulose acetate (CA) films with aligned nanoporous fibers are rolled into a 3D cylinder and partially coated with a carbon black/poly(vinyl alcohol) (CB/PVA) photothermal layer to create an environmentally-friendly SDIE for concurrent desalination and salt recovery. The evaporator achieves a high evaporation rate of 4.44 kg m<sup>−2</sup> h<sup>−1</sup> under 1 sun, corresponding to a photothermal conversion efficiency of 107.3% based on equivalent evaporation enthalpy. This performance is ascribed to reduced vaporization enthalpy from material-water interactions and nanoporous structures, along with cold evaporation-induced environmental energy harvesting. Under 1 sun, the SDIE stably treats brines of 3.5–20 wt% salinity with edge-preferential salt crystallization due to its fibrous microporous architecture. This feature allows gravity-assisted salt collection and durable function in 10 wt% NaCl for 10 days, maintaining average steam generation and salt harvesting rates of 4.71 kg m<sup>−2</sup> h<sup>−1</sup> and 3.21 kg m<sup>−2</sup> day<sup>−1</sup>, respectively. Condensed waters from 3.5 wt% NaCl and simulated seawater exhibit high purity with significantly lower conductivities. The outdoor experiment also reveals the stable performance of the SDIE under actual conditions. Computational fluid dynamics (CFD) simulation further validates edge-preferential salt aggregation. This innovative device offers a promising route for simultaneous freshwater and salt collection from brines.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"12 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146135574","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Due to the presence of high content of oxygenated compounds (aldehydes, alcohols, carboxylic acids, esters, ethers, furfurals, ketones, lignin-derived compounds, phenols, and sugars), bio-oil has inferior oil properties compared to petroleum-derived oils. This creates numerous technological challenges in downstream separation processes. The present study outlines recent research trends on various separation strategies for upgrading crude biogenic pyrolysis oil for the production of valuable commodities. The focus of the present study mainly concentrates on the various separation strategies such as column chromatography, distillation, membrane filtration, crystallization, solvent extraction, electrosorption, and fractional condensation with respect to principles of operation, efficiency, economy and environmental concerns. Phase separation using solvent and adsorbent was found to be the best separation strategy compared to others due to lower capital investment and energy expenditure. However, there are various technological challenges with separation strategies for scale-up in industries. A comparative analysis of various separation strategies with the application of various bio-oil fractions from aqueous phases of bio-oil is summarized to understand the possible pathways for utilization in various industries. A brief section on technoeconomic analysis with existing pilot and semi-pilot pyrolysis plants is presented to understand the economic feasibility of pyrolysis and upgrading strategies. In the end, the circular economy perspective of the pyrolysis-separation and its integration with a machine learning model, are briefly outlined.
{"title":"Recent progress in separation strategies for upgrading bio-oil: mechanisms, challenges and a way forward","authors":"Akhil Mohan, Åsa Emmer, Klas Engvall, Mats Jonsson","doi":"10.1016/j.seppur.2026.137146","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.137146","url":null,"abstract":"Due to the presence of high content of oxygenated compounds (aldehydes, alcohols, carboxylic acids, esters, ethers, furfurals, ketones, lignin-derived compounds, phenols, and sugars), bio-oil has inferior oil properties compared to petroleum-derived oils. This creates numerous technological challenges in downstream separation processes. The present study outlines recent research trends on various separation strategies for upgrading crude biogenic pyrolysis oil for the production of valuable commodities. The focus of the present study mainly concentrates on the various separation strategies such as column chromatography, distillation, membrane filtration, crystallization, solvent extraction, electrosorption, and fractional condensation with respect to principles of operation, efficiency, economy and environmental concerns. Phase separation using solvent and adsorbent was found to be the best separation strategy compared to others due to lower capital investment and energy expenditure. However, there are various technological challenges with separation strategies for scale-up in industries. A comparative analysis of various separation strategies with the application of various bio-oil fractions from aqueous phases of bio-oil is summarized to understand the possible pathways for utilization in various industries. A brief section on technoeconomic analysis with existing pilot and semi-pilot pyrolysis plants is presented to understand the economic feasibility of pyrolysis and upgrading strategies. In the end, the circular economy perspective of the pyrolysis-separation and its integration with a machine learning model, are briefly outlined.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"17 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146115827","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Enhancing the stability of Mn-based ion sieves via high-valence W doping for efficient lithium recovery from seawater","authors":"Enhui Liu, Haiyan Luo, Niankun Jiao, Weitao Zhang, Xin Zhou, Lianying Wu, Haoyu Yao, Xiangfeng Liang, Huizhou Liu","doi":"10.1016/j.seppur.2026.137110","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.137110","url":null,"abstract":"","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"289 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146110311","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-04DOI: 10.1016/j.seppur.2026.137139
Bin Zhao, Bo Zhou, Peidong Zuo, Liping Chang, Mengmeng Wu, Chao Yang, Xu Wu, Zhifeng Qin
{"title":"Deciphering the multistage mechanistic landscape of COS removal by tertiary amines through combined experiments and molecular descriptors","authors":"Bin Zhao, Bo Zhou, Peidong Zuo, Liping Chang, Mengmeng Wu, Chao Yang, Xu Wu, Zhifeng Qin","doi":"10.1016/j.seppur.2026.137139","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.137139","url":null,"abstract":"","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"8 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146110897","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In the development of efficient catalysts for antibiotic degradation, catalyst recovery has long been a major challenge. Immobilizing advanced oxidation catalysts within porous biopolymer supports such as chitosan beads can effectively address this issue, but their cyclic stability remains a key focus of research. In this study, a novel chitosan aerogel microsphere embedded with cobalt‑iron layered double hydroxide (CS/CoFe LDH) was synthesized to efficiently activate peroxymonosulfate (PMS) to degrade tetracycline (TC). The CS/CoFe LDH aerogel microspheres constructed a three-dimensional porous network and contained abundant functional groups, thereby enhancing TC removal and facilitating catalyst recovery. Under optimal conditions, the CS/CoFe/PMS system achieved near-complete degradation of TC. The catalyst maintained high activity at pH 3–11 and in real water environments, with TC removal efficiency remaining above 82% even after five reuse cycles.Mechanistic investigations revealed that TC degradation was predominantly governed by a non-radical oxidation pathway, with superoxide radicals (·O2−) playing an auxiliary role, while hydroxyl radicals (·OH) and sulfate radicals (·SO4−) contributed to a lesser extent, indicating the coexistence of multiple oxidative pathways. The surface redox cycling of Co2+/Co3+ and Fe2+/Fe3+ was identified as the key mechanism for continuous PMS activation. Combined with liquid chromatography-mass spectrometry (LC-MS) and density functional theory (DFT) analysis, key intermediate products were identified, and degradation pathways involving demethylation, hydroxylation, ring cleavage, etc., were proposed. Toxicity predictions indicated that these intermediates were generally less harmful than TC, confirming the safety of the mineralization process. This work provides valuable mechanistic insights and demonstrates the application potential of aerogel-encapsulated LDH catalysts for water remediation and antibiotic removal.
{"title":"Chitosan aerogel beads embedded with CoFe layered double hydroxide for peroxymonosulfate activation","authors":"Wenjun Zeng, Yidan Luo, Shujuan He, Huiyin Ye, Yueyang Xiao, Shuohan Yu, Yu Xie, Mingshan Xue, Zuozhu Yin, Zugen Liu, Bin Gao","doi":"10.1016/j.seppur.2026.137149","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.137149","url":null,"abstract":"In the development of efficient catalysts for antibiotic degradation, catalyst recovery has long been a major challenge. Immobilizing advanced oxidation catalysts within porous biopolymer supports such as chitosan beads can effectively address this issue, but their cyclic stability remains a key focus of research. In this study, a novel chitosan aerogel microsphere embedded with cobalt‑iron layered double hydroxide (CS/CoFe LDH) was synthesized to efficiently activate peroxymonosulfate (PMS) to degrade tetracycline (TC). The CS/CoFe LDH aerogel microspheres constructed a three-dimensional porous network and contained abundant functional groups, thereby enhancing TC removal and facilitating catalyst recovery. Under optimal conditions, the CS/CoFe/PMS system achieved near-complete degradation of TC. The catalyst maintained high activity at pH 3–11 and in real water environments, with TC removal efficiency remaining above 82% even after five reuse cycles.Mechanistic investigations revealed that TC degradation was predominantly governed by a non-radical oxidation pathway, with superoxide radicals (<strong>·O</strong><sub><strong>2</strong></sub><sup>−</sup>) playing an auxiliary role, while hydroxyl radicals (<strong>·OH</strong>) and sulfate radicals (<strong>·SO</strong><sub><strong>4</strong></sub><sup>−</sup>) contributed to a lesser extent, indicating the coexistence of multiple oxidative pathways. The surface redox cycling of Co<sup>2+</sup>/Co<sup>3+</sup> and Fe<sup>2+</sup>/Fe<sup>3+</sup> was identified as the key mechanism for continuous PMS activation. Combined with liquid chromatography-mass spectrometry (LC-MS) and density functional theory (DFT) analysis, key intermediate products were identified, and degradation pathways involving demethylation, hydroxylation, ring cleavage, etc., were proposed. Toxicity predictions indicated that these intermediates were generally less harmful than TC, confirming the safety of the mineralization process. This work provides valuable mechanistic insights and demonstrates the application potential of aerogel-encapsulated LDH catalysts for water remediation and antibiotic removal.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"398 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146115826","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-04DOI: 10.1016/j.seppur.2026.137127
Ming Zhang, Jiacheng Li, Lijun Wu, Tian Liang, Jian Liu, Lu Wang
Acetamiprid (ACE) can accumulate in the environment through the food chain, potentially endanger human health. In this experiment, zinc‑cobalt bimetallic metal organic framework (Zn/Co MOF) was synthesized and used to activate peroxymonosulfate (PMS) for the removal of ACE from water. The degradation efficiency of ACE could achieve approximately 96.93% after 90 min. Through the synergistic effect of Zn and Co bimetallic sites, ACE was degraded via a Fenton-like reaction, while reactive oxygen species (SO4·-, ·OH, O2·-, and 1O2) participated in the process. The high catalytic activity of Zn/Co MOF led to the degradation of ACE through the formation of a series of low-toxicity intermediates, and partial mineralization to CO2 and H2O. In addition, Zn/Co MOF remained effective under broad pH conditions (pH 5–11) and temperatures (5–45 °C). This system had excellent degradation effects in actual water, with degradation rates of 95.42% and 95.18% after 90 min in the Pai River and Liren Lake, respectively. With its high catalytic performance, the Zn/Co MOF is expected to become an ideal catalyst that could be used to remove pesticide residues in water.
{"title":"One-step hydrothermal synthesis of Zn/Co MOF for efficiently activating PMS to degrade organic pollutants in water: The reaction kinetics and mechanism","authors":"Ming Zhang, Jiacheng Li, Lijun Wu, Tian Liang, Jian Liu, Lu Wang","doi":"10.1016/j.seppur.2026.137127","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.137127","url":null,"abstract":"Acetamiprid (ACE) can accumulate in the environment through the food chain, potentially endanger human health. In this experiment, zinc‑cobalt bimetallic metal organic framework (Zn/Co MOF) was synthesized and used to activate peroxymonosulfate (PMS) for the removal of ACE from water. The degradation efficiency of ACE could achieve approximately 96.93% after 90 min. Through the synergistic effect of Zn and Co bimetallic sites, ACE was degraded via a Fenton-like reaction, while reactive oxygen species (SO<sub>4</sub><sup>·-</sup>, ·OH, O<sub>2</sub><sup>·-</sup>, and <sup>1</sup>O<sub>2</sub>) participated in the process. The high catalytic activity of Zn/Co MOF led to the degradation of ACE through the formation of a series of low-toxicity intermediates, and partial mineralization to CO<sub>2</sub> and H<sub>2</sub>O. In addition, Zn/Co MOF remained effective under broad pH conditions (pH 5–11) and temperatures (5–45 °C). This system had excellent degradation effects in actual water, with degradation rates of 95.42% and 95.18% after 90 min in the Pai River and Liren Lake, respectively. With its high catalytic performance, the Zn/Co MOF is expected to become an ideal catalyst that could be used to remove pesticide residues in water.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"83 1","pages":"137127"},"PeriodicalIF":8.6,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146135564","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-03DOI: 10.1016/j.seppur.2026.137138
Roberta Y.N. Reis, Alberto Rodríguez-Gómez, Caio V.S. Almeida, Lucia H. Mascaro, Manuel A. Rodrigo
Hydrogen sulfide (H2S) is a highly toxic and corrosive gas commonly found in industrial emissions, posing serious environmental and operational risks. This work proposes an innovative photoelectrocatalytic strategy for the simultaneous degradation of gaseous H2S and the generation of green hydrogen (H2) under flux conditions. The system integrates gas-liquid absorption with electrochemical and photoelectrochemical oxidation, employing a WO3 photoanode and a stainless steel cathode separated by a proton exchange membrane. The performance of the electrocatalytic and photoelectrocatalytic configurations was systematically evaluated regarding H2S removal efficiency, hydrogen production, and energy consumption. The photoelectrocatalytic process exhibited superior activity, achieving a degradation of 8.2 mg S with a Coulombic efficiency of 3600 mg S Ah−1 for H2S oxidation and a Faradaic efficiency of 60% for H2 evolution at an applied current density of 0.33 mA cm−2. Illumination with a 10 W high-power blue LED significantly increased charge separation and reduced the cell potential, resulting in higher energy efficiency. Post-reaction characterization by X-ray photoelectron spectroscopy (XPS) demonstrated partial sulfur deposition on the WO3 surface and the presence of oxidized sulfur species. Overall, the results demonstrate that photoelectrocatalysis under optimized conditions offers an efficient and sustainable route for simultaneous H2S reduction and hydrogen generation, providing a promising dual-purpose platform for environmental remediation and renewable energy production.
硫化氢(H2S)是一种剧毒腐蚀性气体,常见于工业排放中,具有严重的环境和操作风险。这项工作提出了一种创新的光电催化策略,用于在通量条件下同时降解气态H2S和生成绿色氢(H2)。该系统将气液吸收与电化学和光电化学氧化相结合,采用WO3光阳极和由质子交换膜分离的不锈钢阴极。系统地评估了电催化和光催化构型对H2S的去除效率、产氢量和能耗。光电催化过程表现出优异的活性,在0.33 mA cm−2的电流密度下,H2S氧化的库仑效率为3600 mg S Ah−1,降解8.2 mg S,氢气析出的法拉第效率为60%。10 W高功率蓝色LED的照明显著增加了电荷分离,降低了电池电位,从而提高了能源效率。反应后的x射线光电子能谱(XPS)表征表明,WO3表面有部分硫沉积,并且存在氧化硫。综上所述,优化条件下的光电催化为同时还原H2S和制氢提供了一条高效、可持续的途径,为环境修复和可再生能源生产提供了一个有前景的双用途平台。
{"title":"Enhancing hydrogen sulfide removal through photoelectrochemistry with WO3 photoanodes under blue LED irradiation","authors":"Roberta Y.N. Reis, Alberto Rodríguez-Gómez, Caio V.S. Almeida, Lucia H. Mascaro, Manuel A. Rodrigo","doi":"10.1016/j.seppur.2026.137138","DOIUrl":"https://doi.org/10.1016/j.seppur.2026.137138","url":null,"abstract":"Hydrogen sulfide (H<sub>2</sub>S) is a highly toxic and corrosive gas commonly found in industrial emissions, posing serious environmental and operational risks. This work proposes an innovative photoelectrocatalytic strategy for the simultaneous degradation of gaseous H<sub>2</sub>S and the generation of green hydrogen (H<sub>2</sub>) under flux conditions. The system integrates gas-liquid absorption with electrochemical and photoelectrochemical oxidation, employing a WO<sub>3</sub> photoanode and a stainless steel cathode separated by a proton exchange membrane. The performance of the electrocatalytic and photoelectrocatalytic configurations was systematically evaluated regarding H<sub>2</sub>S removal efficiency, hydrogen production, and energy consumption. The photoelectrocatalytic process exhibited superior activity, achieving a degradation of 8.2 mg S with a Coulombic efficiency of 3600 mg S Ah<sup>−1</sup> for H<sub>2</sub>S oxidation and a Faradaic efficiency of 60% for H<sub>2</sub> evolution at an applied current density of 0.33 mA cm<sup>−2</sup>. Illumination with a 10 W high-power blue LED significantly increased charge separation and reduced the cell potential, resulting in higher energy efficiency. Post-reaction characterization by X-ray photoelectron spectroscopy (XPS) demonstrated partial sulfur deposition on the WO<sub>3</sub> surface and the presence of oxidized sulfur species. Overall, the results demonstrate that photoelectrocatalysis under optimized conditions offers an efficient and sustainable route for simultaneous H<sub>2</sub>S reduction and hydrogen generation, providing a promising dual-purpose platform for environmental remediation and renewable energy production.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"5 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101344","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}