Pub Date : 2025-01-22DOI: 10.1016/j.seppur.2025.131746
Jingxuan Yang, Yingjie Li, Huaying Liu, Xiaoning Tang, Huan Li
Developing efficient catalytic antimicrobial materials is crucial for mitigating air microbial pollution. In this study, a monolayer Bi2MoO6 with a unique [BiO]+–[MoO4]2−–[BiO]+ interlayer substructure and “Bi–O” vacancy defects was synthesized through a simple exfoliation method using cetyltrimethylammonium bromide. These monolayers are chemically bonded to form a layered heterojunction. Under solar irradiation, holes are generated in the [BiO]+ layer, while electrons are produced in the [MoO4]2− layer, thereby facilitating efficient direct electron–hole separation. Additionally, the abundant “Bi–O” vacancy defects in the [BiO]+ layer result in crystal structure distortion, electron redistribution, and changes in the band gap energy of Bi2MoO6. The combination of layered heterostructures and vacancy defects significantly enhances solar light utilization and promotes photogenerated carrier separation, leading to excellent photocatalytic antimicrobial performance. Antibacterial tests reveal that after 20 min of irradiation, the monolayer Bi2MoO6 (0.20 mg/mL) deactivates 96.7 % of Escherichia coli and 74.5 % of Staphylococcus aureus. Notably, the antibacterial efficiency of the monolayer Bi2MoO6 is 1.9 and 2.7 times that of its multilayer counterpart for Escherichia coli and Staphylococcus aureus, respectively. This study provides novel insights and strategies for designing layered heterojunction Bi2MoO6 with enhanced photocatalytic antibacterial efficiency and tailored surface defects.
{"title":"Synergistic effects of monolayer Bi2MoO6 layered heterojunctions configuration and surface “Bi–O” vacancy defects of in enhanced photocatalytic antimicrobial performance","authors":"Jingxuan Yang, Yingjie Li, Huaying Liu, Xiaoning Tang, Huan Li","doi":"10.1016/j.seppur.2025.131746","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131746","url":null,"abstract":"Developing efficient catalytic antimicrobial materials is crucial for mitigating air microbial pollution. In this study, a monolayer Bi<sub>2</sub>MoO<sub>6</sub> with a unique [BiO]<sup>+</sup>–[MoO<sub>4</sub>]<sup>2−</sup>–[BiO]<sup>+</sup> interlayer substructure and “Bi–O” vacancy defects was synthesized through a simple exfoliation method using cetyltrimethylammonium bromide. These monolayers are chemically bonded to form a layered heterojunction. Under solar irradiation, holes are generated in the [BiO]<sup>+</sup> layer, while electrons are produced in the [MoO<sub>4</sub>]<sup>2−</sup> layer, thereby facilitating efficient direct electron–hole separation. Additionally, the abundant “Bi–O” vacancy defects in the [BiO]<sup>+</sup> layer result in crystal structure distortion, electron redistribution, and changes in the band gap energy of Bi<sub>2</sub>MoO<sub>6</sub>. The combination of layered heterostructures and vacancy defects significantly enhances solar light utilization and promotes photogenerated carrier separation, leading to excellent photocatalytic antimicrobial performance. Antibacterial tests reveal that after 20 min of irradiation, the monolayer Bi<sub>2</sub>MoO<sub>6</sub> (0.20 mg/mL) deactivates 96.7 % of <em>Escherichia coli</em> and 74.5 % of <em>Staphylococcus aureus</em>. Notably, the antibacterial efficiency of the monolayer Bi<sub>2</sub>MoO<sub>6</sub> is 1.9 and 2.7 times that of its multilayer counterpart for <em>Escherichia coli</em> and <em>Staphylococcus aureus</em>, respectively. This study provides novel insights and strategies for designing layered heterojunction Bi<sub>2</sub>MoO<sub>6</sub> with enhanced photocatalytic antibacterial efficiency and tailored surface defects.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"70 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991894","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}
High-flux loose nanofiltration membranes (LNMs) are ideal for treating and recovering dyes and salts from saline textile wastewater. In this study, a self-synthesized polyphenolic monomer (HCTT) was introduced into an interfacial polymerization (IP) system, establishing a dual physical and chemical constraint mechanism to regulate the reaction rate. Physically, HCTT exhibits a slow diffusion rate and reduces the diffusion rate of piperazine (PIP). Chemically, the phenolic hydroxyl groups of HCTT are less reactive than the amino groups of PIP, enhancing the controllability of the IP process. Using HCTT and anhydrous PIP as the aqueous phase and trimesoylchloride (TMC) as the oil phase, LNMs were prepared on hydrolyzed polyacrylonitrile (HPAN) substrates. The resulting membranes feature a negatively charged hydrophilic surface and a selective layer with a Turing structure, improving water permeability and mass transfer. The membranes achieved a flux of 124.8 LMH bar−1 with dye rejection rates exceeding 95 % for Congo Red (CR) and Methyl Violet (MV) while maintaining low salt rejection rates (14.1 % for Na2SO4 and 5.4 % for MgSO4), resulting in a dye/salt selectivity 14.9 times higher than conventional polyamide membranes. The membranes demonstrated excellent performance in mixed dye/salt solutions and maintained high stability after 48 h of continuous operation, achieving a flux recovery rate of 84.2 % after seven fouling cycles with CR. This study offers a novel and efficient strategy for developing LNMs for dye containing wastewater treatment and resource recovery.
{"title":"Preparation of high-flux loose nanofiltration membranes for efficient dye/salt separation by controlling interface polymerization through physical and chemical dual constraints","authors":"Haoshuo Li, Shujuan Xiao, Xiang Zhao, Jianguo Yuan, Shouwu Yu","doi":"10.1016/j.seppur.2025.131720","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131720","url":null,"abstract":"High-flux loose nanofiltration membranes (LNMs) are ideal for treating and recovering dyes and salts from saline textile wastewater. In this study, a self-synthesized polyphenolic monomer (HCTT) was introduced into an interfacial polymerization (IP) system, establishing a dual physical and chemical constraint mechanism to regulate the reaction rate. Physically, HCTT exhibits a slow diffusion rate and reduces the diffusion rate of piperazine (PIP). Chemically, the phenolic hydroxyl groups of HCTT are less reactive than the amino groups of PIP, enhancing the controllability of the IP process. Using HCTT and anhydrous PIP as the aqueous phase and trimesoylchloride (TMC) as the oil phase, LNMs were prepared on hydrolyzed polyacrylonitrile (HPAN) substrates. The resulting membranes feature a negatively charged hydrophilic surface and a selective layer with a Turing structure, improving water permeability and mass transfer. The membranes achieved a flux of 124.8 LMH bar<sup>−1</sup> with dye rejection rates exceeding 95 % for Congo Red (CR) and Methyl Violet (MV) while maintaining low salt rejection rates (14.1 % for Na<sub>2</sub>SO<sub>4</sub> and 5.4 % for MgSO<sub>4</sub>), resulting in a dye/salt selectivity 14.9 times higher than conventional polyamide membranes. The membranes demonstrated excellent performance in mixed dye/salt solutions and maintained high stability after 48 h of continuous operation, achieving a flux recovery rate of 84.2 % after seven fouling cycles with CR. This study offers a novel and efficient strategy for developing LNMs for dye containing wastewater treatment and resource recovery.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"11 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142992213","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131685
Yilong Zhu, Huifang Xing, Shan Ni, Ke Xu, ZhaoXiang Zhong, Liangrong Yang
The recycling of precious materials, such as palladium (Pd), was repeatedly documented as essential for a sustainable future with respect to the environment and energy production. However, high-efficiency extraction presented significant challenges. In this work, a surface hydroxyl regulation strategy was used to prepare a defective carbon nitride (CN) with a high specific surface area and hierarchical porosity through cobalt (Co)-doping. Characterization confirmed the successful synthesis of the adsorbent. The results indicated that the optimal pH for the adsorption process was 5.5, adsorption kinetics and isotherms of Pd on the adsorbent suggested that the adsorption followed a pseudo-second-order model and the Langmuir model, respectively. The maximum adsorption capacity reached up to 529.1 mg·g–1. In addition, it showed high affinity for Pd ions, the Kd value was 4.1 × 104 ml·g–1. After Pd adsorption, due to the presence of abundant and uniformly dispersed Pd and Co particles which further facilitated cooperative catalysis on the surface of adsorbent, As a result, the Co-CN-Pd was reused as a catalyst for p-nitrophenol hydrogenation. It achieved a turnover frequency (TOF) as high as 1032.6 h–1, significantly surpassing other catalysts reported in the literature. Overall, this novel adsorbent presented broad application prospects in the field of Pd recovery and reuse.
{"title":"Recovery of palladium from solution by defective Carbon nitride and Regenerating as a hydrogenation catalysis","authors":"Yilong Zhu, Huifang Xing, Shan Ni, Ke Xu, ZhaoXiang Zhong, Liangrong Yang","doi":"10.1016/j.seppur.2025.131685","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131685","url":null,"abstract":"The recycling of precious materials, such as palladium (Pd), was repeatedly documented as essential for a sustainable future with respect to the environment and energy production. However, high-efficiency extraction presented significant challenges. In this work, a surface hydroxyl regulation strategy was used to prepare a defective carbon nitride (CN) with a high specific surface area and hierarchical porosity through cobalt (Co)-doping. Characterization confirmed the successful synthesis of the adsorbent. The results indicated that the optimal pH for the adsorption process was 5.5, adsorption kinetics and isotherms of Pd on the adsorbent suggested that the adsorption followed a pseudo-second-order model and the Langmuir model, respectively. The maximum adsorption capacity reached up to 529.1 mg·g<sup>–1</sup>. In addition, it showed high affinity for Pd ions, the <em>K<sub>d</sub></em> value was 4.1 × 10<sup>4</sup> ml·g<sup>–1</sup>. After Pd adsorption, due to the presence of abundant and uniformly dispersed Pd and Co particles which further facilitated cooperative catalysis on the surface of adsorbent, As a result, the Co-CN-Pd was reused as a catalyst for p-nitrophenol hydrogenation. It achieved a turnover frequency (TOF) as high as 1032.6 h<sup>–1</sup>, significantly surpassing other catalysts reported in the literature. Overall, this novel adsorbent presented broad application prospects in the field of Pd recovery and reuse.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"9 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991891","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131724
Marek Wasilewski, Grzegorz Ligus, Lakhbir Singh Brar
This research investigates the impact of various prismatic heights (PHs) on the performance of square cyclones at three Reynolds numbers, viz. Re = 27626, 37,985 and 48345. We have accounted for seven different PHs, viz. 1.0D, 1.5D, 2.0D, 2.5D, 3.0D, 3.5D, and 4.0D – here, D represents the prismatic section dimension of the square cross-sectional area. Model 2.0D is the reference model used to evaluate relative performance. A high-performance turbulence model large-eddy simulation has been used to calculate the separation efficiency and pressure drop. The assumptions made in the numerical studies were validated using experimental and PIV studies. Considering the latter, solid particles with three different densities viz. 1100, 2100, and 2800 kg/m3 are analysed. We also present the flow details in the form of variations in the mean and standard deviation values of scalar and vector quantities. It has been observed that with an increase in the PH, given a Re value, there is a marginal variation in pressure drop values, which amounts to a maximum value of less than 5 % at Re = 48345. Compared to the mild variations in pressure losses, the differences in the collection efficiencies are significant but slightly dramatic (in context to the particle density). A maximum enhancement of more than 26 % has been observed for particle density 1100 kg/m3 at Re = 48345. Conclusive results indicate that model 4.0D outperforms all the variants, and this model works more efficiently, particularly for low-density particles. It was shown that in the case of square cyclones, it may also be important to adapt the geometry of the separator not only to the flow conditions of the fluid phase but also to take into account the properties of the solid phase. In this case, the selection of PHs may be crucial.
{"title":"Investigations of the flow phenomena inside square cyclone separators with different prismatic heights","authors":"Marek Wasilewski, Grzegorz Ligus, Lakhbir Singh Brar","doi":"10.1016/j.seppur.2025.131724","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131724","url":null,"abstract":"This research investigates the impact of various prismatic heights (PHs) on the performance of square cyclones at three Reynolds numbers, viz. <em>Re</em> = 27626, 37,985 and 48345. We have accounted for seven different PHs, viz. 1.0<em>D</em>, 1.5<em>D</em>, 2.0<em>D</em>, 2.5<em>D</em>, 3.0<em>D</em>, 3.5<em>D</em>, and 4.0<em>D</em> – here, <em>D</em> represents the prismatic section dimension of the square cross-sectional area. Model 2.0<em>D</em> is the reference model used to evaluate relative performance. A high-performance turbulence model large-eddy simulation has been used to calculate the separation efficiency and pressure drop. The assumptions made in the numerical studies were validated using experimental and PIV studies. Considering the latter, solid particles with three different densities viz. 1100, 2100, and 2800 kg/m<sup>3</sup> are analysed. We also present the flow details in the form of variations in the mean and standard deviation values of scalar and vector quantities. It has been observed that with an increase in the PH, given a <em>Re</em> value, there is a marginal variation in pressure drop values, which amounts to a maximum value of less than 5 % at <em>Re</em> = 48345. Compared to the mild variations in pressure losses, the differences in the collection efficiencies are significant but slightly dramatic (in context to the particle density). A maximum enhancement of more than 26 % has been observed for particle density 1100 kg/m<sup>3</sup> at <em>Re</em> = 48345. Conclusive results indicate that model 4.0<em>D</em> outperforms all the variants, and this model works more efficiently, particularly for low-density particles. It was shown that in the case of square cyclones, it may also be important to adapt the geometry of the separator not only to the flow conditions of the fluid phase but also to take into account the properties of the solid phase. In this case, the selection of PHs may be crucial.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"49 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142992211","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131739
Yujie Tan, Minghui Sun, Shi Zhou, Mifan Wang, Fuqiang Huo, Bin Su, Bo Liu, Wei Jiang, Chunbo Liu
Developing a Fenton-like peroxymonosulfate (PMS) activator capable of producing 1O2 is beneficial for treating high-salinity wastewater. Herein, the FeTCPP-CN catalyst was synthesized by self-assembling iron (Ⅲ) tetrakis(4-carboxyphenyl)porphyrin (FeTCPP) molecule with lamellar carbon nitride (CN) polymer. The formed hydrophilic-hydrophobic heterointerface enhanced the adsorption potential with pollutants, and the hydrogen bonding and π-π interactions between interfaces constructed an efficient electron transfer channel, while the highly dispersed Fe-N4 moiety promoted atomic utilization efficiency. In the FeTCPP-CN/PMS system, 2,4-dichlorophenol (2,4-DCP) could be efficiently degraded under high concentration (200 mM) of inorganic salts, and the excellent degradation performance could be maintained over 10 cycles in a continuous flow device. During the reaction, the O2·- and 1O2 were identified as the main active species, where *SO5·- was the crucial intermediate to selectively generate 1O2. This work offers insights into the construction of efficient catalysts for the treatment of high-salinity phenolic wastewater.
{"title":"Self-assembled metalloporphyrin-carbon nitride heterointerface promotes fenton-like activity to purify high-salinity phenolic wastewater","authors":"Yujie Tan, Minghui Sun, Shi Zhou, Mifan Wang, Fuqiang Huo, Bin Su, Bo Liu, Wei Jiang, Chunbo Liu","doi":"10.1016/j.seppur.2025.131739","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131739","url":null,"abstract":"Developing a Fenton-like peroxymonosulfate (PMS) activator capable of producing <sup>1</sup>O<sub>2</sub> is beneficial for treating high-salinity wastewater. Herein, the FeTCPP-CN catalyst was synthesized by self-assembling iron (Ⅲ) tetrakis(4-carboxyphenyl)porphyrin (FeTCPP) molecule with lamellar carbon nitride (CN) polymer. The formed hydrophilic-hydrophobic heterointerface enhanced the adsorption potential with pollutants, and the hydrogen bonding and π-π interactions between interfaces constructed an efficient electron transfer channel, while the highly dispersed Fe-N<sub>4</sub> moiety promoted atomic utilization efficiency. In the FeTCPP-CN/PMS system, 2,4-dichlorophenol (2,4-DCP) could be efficiently degraded under high concentration (200 mM) of inorganic salts, and the excellent degradation performance could be maintained over 10 cycles in a continuous flow device. During the reaction, the O<sub>2</sub><strong><sup>·</sup></strong><sup>-</sup> and <sup>1</sup>O<sub>2</sub> were identified as the main active species, where *SO<sub>5</sub><strong><sup>·</sup></strong><sup>-</sup> was the crucial intermediate to selectively generate <sup>1</sup>O<sub>2</sub>. This work offers insights into the construction of efficient catalysts for the treatment of high-salinity phenolic wastewater.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"14 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991899","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}
Manganese oxide (MnOx) catalysts are promising for low-temperature NH3-Selective Catalytic Reduction (NH3-SCR) with their superior catalytic performance. However, the presence of alkali metals in flue gases, particularly potassium (K), leads to catalyst deactivation and limits their industrial application. This study investigates the synergistic effects of Ce and Nb doping on the K resistance and low-temperature NH3-SCR activity of MnOx. The surface acidity and redox properties of MnOx were modulated by Ce and Nb modification. In addition, the phase structure, surface state and active sites of the catalysts were characterized before and after K poisoning. The results indicated that Nb0.05Ce0.05MnOx exhibited exceptional low-temperature performance, achieving over 90 % NO conversion at 125-250°C, along with significant resistance to K poisoning·NH3-TPD and in-situ experiments revealed that the loss of acid sites is the primary cause of K poisoning. The mechanism follows the L-H mechanism with L-acid sites as the main active sites on the catalyst surface and bridging nitrate as the key intermediate state. This research provides valuable insights into enhancing the industrial applicability of MnOx-based catalysts for low-temperature denitrification.
{"title":"Enhancing the K-resistance of MnOx catalysts via Ce and Nb co-doping for low-temperature NOx elimination","authors":"Yanping Yang, Shengchen Li, Shunli Shi, Jie Hu, Zexi Xuchen, Shunmin Ding, Dan zhao, Shengjun Deng, Weiming Xiao, Shuhua Wang, Chao Chen","doi":"10.1016/j.seppur.2025.131768","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131768","url":null,"abstract":"Manganese oxide (MnO<sub>x</sub>) catalysts are promising for low-temperature NH<sub>3</sub>-Selective Catalytic Reduction (NH<sub>3</sub>-SCR) with their superior catalytic performance. However, the presence of alkali metals in flue gases, particularly potassium (K), leads to catalyst deactivation and limits their industrial application. This study investigates the synergistic effects of Ce and Nb doping on the K resistance and low-temperature NH<sub>3</sub>-SCR activity of MnO<sub>x</sub>. The surface acidity and redox properties of MnO<sub>x</sub> were modulated by Ce and Nb modification. In addition, the phase structure, surface state and active sites of the catalysts were characterized before and after K poisoning. The results indicated that Nb<sub>0.05</sub>Ce<sub>0.05</sub>MnO<sub>x</sub> exhibited exceptional low-temperature performance, achieving over 90 % NO conversion at 125-250°C, along with significant resistance to K poisoning·NH<sub>3</sub>-TPD and <em>in-situ</em> experiments revealed that the loss of acid sites is the primary cause of K poisoning. The mechanism follows the L-H mechanism with L-acid sites as the main active sites on the catalyst surface and bridging nitrate as the key intermediate state. This research provides valuable insights into enhancing the industrial applicability of MnO<sub>x-</sub>based catalysts for low-temperature denitrification.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"1 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020900","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131738
Cheng Peng, Qiongfang Wang, Xin Zhang, Lei Dong, Yulin Yuan, Min Zhang, Pinhua Rao, Naiyun Gao, Jing Deng
In the activation of peroxymonosulfate by transition metal catalysts, manipulating the formation of high-valent metals facilitates the efficient utilization of persulfates and the removal of organic pollutants. Additionally, the synergistic effect between bimetallic catalysts has been demonstrated to be more advantageous for persulfate activation. In this research, the Co2(OH)2CO3/CuCo2S4 (COC/CCS) composite catalyst was successfully prepared by loading CuCo2S4 onto Co2(OH)2CO3 using a one-step method. Experimental results showed that the COC/CCS/PMS system could mediate the efficient degradation of various antibiotics through the synergistic action of multiple reactive species, predominantly high-valent metals [Co(IV) = Oxo and Cu(III)], SO4•−, and 1O2. The larger average pore size and pore volume of COC/CCS exposed more active sites. At the Co active sites, PMS underwent a two-electron transfer to form Co(IV) = Oxo. The Cu active sites played different roles depending on the pH: under acidic conditions, PMS served as an electron donor, transferring electrons to COC/CCS, which favored the reduction of Cu(II) and promoted the Co/Cu bimetallic cycle. Under neutral (alkaline) conditions, the generation of Cu(III) was induced, accelerating the degradation reaction. Additionally, the COC/CCS/PMS system exhibited significant resistance to anions, humic acid, and pH interference, and exhibited superior catalytic performance in actual water conditions. After four cycles, sulfachloropyridazine (SCP) was still completely degraded within 30 min, and the degradation pathway of SCP and the toxicity of the intermediate products were analyzed. This research provided insights into the interaction between bimetallic catalyst active sites and PMS, and the generation of high-valent metals to degrade antibiotics.
在过渡金属催化剂活化过氧单硫酸盐的过程中，操纵高价金属的形成有利于过硫酸盐的高效利用和有机污染物的去除。此外，双金属催化剂之间的协同作用更有利于过硫酸盐的活化。本研究通过一步法将CuCo2S4装载到Co2(OH)2CO3上，成功制备了Co2(OH)2CO3/CuCo2S4 （COC/CCS）复合催化剂。实验结果表明，COC/CCS/PMS系统可以通过多种活性物质的协同作用，介导多种抗生素的高效降解，主要是高价金属[Co（IV） = Oxo and Cu(III)]、SO4•−和1O2。COC/CCS的平均孔径和孔体积越大，暴露的活性位点越多。在Co活性位点，PMS发生双电子转移形成Co（IV） = Oxo。Cu活性位点的作用随pH的不同而不同：在酸性条件下，PMS作为电子供体，将电子转移到COC/CCS，有利于Cu（II）的还原，促进Co/Cu双金属循环；在中性（碱性）条件下，诱导Cu（III）的生成，加速降解反应。此外，COC/CCS/PMS体系对阴离子、腐植酸和pH干扰具有显著的抗性，在实际水条件下表现出优异的催化性能。4个循环后，磺胺氯吡嗪（SCP）在30 min内仍能完全降解，并对SCP的降解途径及中间产物的毒性进行了分析。本研究为双金属催化剂活性位点与PMS之间的相互作用以及高价金属降解抗生素的产生提供了见解。
{"title":"Efficient degradation of SCP by Co2(OH)2CO3/CuCo2S4-enhanced electron transfer-activated PMS: Dual role of Cu active site","authors":"Cheng Peng, Qiongfang Wang, Xin Zhang, Lei Dong, Yulin Yuan, Min Zhang, Pinhua Rao, Naiyun Gao, Jing Deng","doi":"10.1016/j.seppur.2025.131738","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131738","url":null,"abstract":"In the activation of peroxymonosulfate by transition metal catalysts, manipulating the formation of high-valent metals facilitates the efficient utilization of persulfates and the removal of organic pollutants. Additionally, the synergistic effect between bimetallic catalysts has been demonstrated to be more advantageous for persulfate activation. In this research, the Co<sub>2</sub>(OH)<sub>2</sub>CO<sub>3</sub>/CuCo<sub>2</sub>S<sub>4</sub> (COC/CCS) composite catalyst was successfully prepared by loading CuCo<sub>2</sub>S<sub>4</sub> onto Co<sub>2</sub>(OH)<sub>2</sub>CO<sub>3</sub> using a one-step method. Experimental results showed that the COC/CCS/PMS system could mediate the efficient degradation of various antibiotics through the synergistic action of multiple reactive species, predominantly high-valent metals [Co(IV) = Oxo and Cu(III)], SO<sub>4</sub><sup>•−</sup>, and <sup>1</sup>O<sub>2</sub>. The larger average pore size and pore volume of COC/CCS exposed more active sites. At the Co active sites, PMS underwent a two-electron transfer to form Co(IV) = Oxo. The Cu active sites played different roles depending on the pH: under acidic conditions, PMS served as an electron donor, transferring electrons to COC/CCS, which favored the reduction of Cu(II) and promoted the Co/Cu bimetallic cycle. Under neutral (alkaline) conditions, the generation of Cu(III) was induced, accelerating the degradation reaction. Additionally, the COC/CCS/PMS system exhibited significant resistance to anions, humic acid, and pH interference, and exhibited superior catalytic performance in actual water conditions. After four cycles, sulfachloropyridazine (SCP) was still completely degraded within 30 min, and the degradation pathway of SCP and the toxicity of the intermediate products were analyzed. This research provided insights into the interaction between bimetallic catalyst active sites and PMS, and the generation of high-valent metals to degrade antibiotics.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"59 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142992619","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131749
Jie Wu, Zhengyang Jiang, Hancheng Xie, Jinlong Fan, Yaoyin Lou, Jian Liu, Shaohua Chen, Yaoxing Liu, Xin Ye
Developing an effective resource utilization approach for ultraviolet stabilizer (UVS) wastewater is challenging due to its high-salinity and complex organic pollutants. This study employed bipolar membrane electrodialysis (BMED) to reclaim acid and base from actual UVS wastewater. To alleviate potential membrane fouling caused by specific UVS organics, an innovative two-stage pH control strategy and its mechanisms were developed. Results indicate that pH regulation is crucial for the stable operation of a 3.6 kg/d on-site pilot-scale BMED system. Under optimal conditions of current density (40 mA/cm2), initial acid-base concentration (0.02 mol/L), and initial volume ratio (2:2:1), high concentrations of 1.03 mol/L acid and 1.90 mol/L base can be reclaimed with low energy consumption. Analysis of membrane surface morphology, hydrophobicity, and resistance, along with the distribution of organic substances, shows that the two-stage pH regulation reduces fouling by probably minimizing electromigration, aggregation, hydrophobic interaction, adsorption, and deposition of humic- and tryptophan-like substances. Compared to conventional initial pH adjustments, the two-stage pH regulation approach stabilizes acid/base production while reducing process costs to $1.5/kg acid and $1.0/kg base. A life cycle cost analysis reveals that, at a BMED treatment capacity of 20 m3/d, savings of up to $774.7 thousand can be realized over a 3-year lifespan, with a relative payback period of 1.2 years. These findings highlight that BMED coupled with two-stage pH regulation is effective for the acid and base reclamation from UVS wastewater, offering a practical solution for sustainable resource recovery and achieving zero wastewater discharge.
{"title":"An innovative pH control strategy for alleviating membrane fouling in bipolar membrane electrodialysis during ultraviolet stabilizer production wastewater treatment","authors":"Jie Wu, Zhengyang Jiang, Hancheng Xie, Jinlong Fan, Yaoyin Lou, Jian Liu, Shaohua Chen, Yaoxing Liu, Xin Ye","doi":"10.1016/j.seppur.2025.131749","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131749","url":null,"abstract":"Developing an effective resource utilization approach for ultraviolet stabilizer (UVS) wastewater is challenging due to its high-salinity and complex organic pollutants. This study employed bipolar membrane electrodialysis (BMED) to reclaim acid and base from actual UVS wastewater. To alleviate potential membrane fouling caused by specific UVS organics, an innovative two-stage pH control strategy and its mechanisms were developed. Results indicate that pH regulation is crucial for the stable operation of a 3.6 kg/d on-site pilot-scale BMED system. Under optimal conditions of current density (40 mA/cm<sup>2</sup>), initial acid-base concentration (0.02 mol/L), and initial volume ratio (2:2:1), high concentrations of 1.03 mol/L acid and 1.90 mol/L base can be reclaimed with low energy consumption. Analysis of membrane surface morphology, hydrophobicity, and resistance, along with the distribution of organic substances, shows that the two-stage pH regulation reduces fouling by probably minimizing electromigration, aggregation, hydrophobic interaction, adsorption, and deposition of humic- and tryptophan-like substances. Compared to conventional initial pH adjustments, the two-stage pH regulation approach stabilizes acid/base production while reducing process costs to $1.5/kg acid and $1.0/kg base. A life cycle cost analysis reveals that, at a BMED treatment capacity of 20 m<sup>3</sup>/d, savings of up to $774.7 thousand can be realized over a 3-year lifespan, with a relative payback period of 1.2 years. These findings highlight that BMED coupled with two-stage pH regulation is effective for the acid and base reclamation from UVS wastewater, offering a practical solution for sustainable resource recovery and achieving zero wastewater discharge.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"52 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020898","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131745
Xuelin Shi, Zihao Yan, Tong Zhu, Zhirong Sun
To address the issue of insufficient oxygen activation by electrode materials in electro-Fenton-like technology, we prepared a novel composite by one-step electrodeposition on graphite felt (GF) followed by calcination. The CuO@Co3O4/GF composite possessed oxygen vacancies and a heterostructure, which effectively modulated the catalyst’s charge distribution, facilitating oxygen adsorption and activation. The heterostructure enhanced the interfacial electron transfer between CuO and Co3O4, shifting the Co d-band center to higher energies and increasing its electron density, which reduced the oxygen adsorption energy barrier. The presence of oxygen vacancies reduced the kinetic barriers of the oxygen reduction reaction and provided additional active sites. CuO@Co3O4/GF was utilized for chloroquine phosphate degradation, achieving 100 % removal within 60 min, with a reaction rate 5.6 times higher than that of GF, and exhibited exceptional stability and applicability over a broad pH range. This study presents a facile approach for preparing composites with both oxygen vacancies and heterostructures, providing new insights into enhancing electrocatalytic performance.
{"title":"Enhanced activation of molecular oxygen for efficient chloroquine phosphate degradation with CuO@Co3O4/GF heterostructure: Promoting mechanisms of oxygen vacancy and interfacial electronic engineering","authors":"Xuelin Shi, Zihao Yan, Tong Zhu, Zhirong Sun","doi":"10.1016/j.seppur.2025.131745","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131745","url":null,"abstract":"To address the issue of insufficient oxygen activation by electrode materials in electro-Fenton-like technology, we prepared a novel composite by one-step electrodeposition on graphite felt (GF) followed by calcination. The CuO@Co<sub>3</sub>O<sub>4</sub>/GF composite possessed oxygen vacancies and a heterostructure, which effectively modulated the catalyst’s charge distribution, facilitating oxygen adsorption and activation. The heterostructure enhanced the interfacial electron transfer between CuO and Co<sub>3</sub>O<sub>4</sub>, shifting the Co d-band center to higher energies and increasing its electron density, which reduced the oxygen adsorption energy barrier. The presence of oxygen vacancies reduced the kinetic barriers of the oxygen reduction reaction and provided additional active sites. CuO@Co<sub>3</sub>O<sub>4</sub>/GF was utilized for chloroquine phosphate degradation, achieving 100 % removal within 60 min, with a reaction rate 5.6 times higher than that of GF, and exhibited exceptional stability and applicability over a broad pH range. This study presents a facile approach for preparing composites with both oxygen vacancies and heterostructures, providing new insights into enhancing electrocatalytic performance.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"38 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991892","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131748
Kelly M. Conway, Baoxia Mi
Sacrificial membranes typically contain a regenerable surface layer that is designed to address one or more of the critical limitations of membrane separation, such as fouling, low chlorine resistance, and poor selectivity towards certain contaminants. By enabling in-situ removal of fouled, damaged, or spent surface layers, regeneration of the sacrificial membrane can be achieved by depositing a fresh surface layer on the base membrane. In this review, we first review the materials that are currently being studied and evaluated for sacrificial membrane applications and identify new promising materials. Then, we discuss the application of sacrificial membranes to control fouling, increase chlorine resistance, and improve targeted contaminant removal. In particular, we discuss the promise of sacrificial multi-functional membranes that utilize functional materials to remove contaminants by adsorption or reaction simultaneously during filtration. Finally, we conclude with a discussion of regeneration strategies for sacrificial membranes and an outlook on opportunities and challenges in the field. The most promising regeneration strategies for removing spent layers and redepositing new ones are the in-situ procedures that align with the routine cleaning protocols widely adopted by the membrane industry.
{"title":"Sacrificial membranes in water purification: Concepts, current status, and outlook","authors":"Kelly M. Conway, Baoxia Mi","doi":"10.1016/j.seppur.2025.131748","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131748","url":null,"abstract":"Sacrificial membranes typically contain a regenerable surface layer that is designed to address one or more of the critical limitations of membrane separation, such as fouling, low chlorine resistance, and poor selectivity towards certain contaminants. By enabling in-situ removal of fouled, damaged, or spent surface layers, regeneration of the sacrificial membrane can be achieved by depositing a fresh surface layer on the base membrane. In this review, we first review the materials that are currently being studied and evaluated for sacrificial membrane applications and identify new promising materials. Then, we discuss the application of sacrificial membranes to control fouling, increase chlorine resistance, and improve targeted contaminant removal. In particular, we discuss the promise of sacrificial multi-functional membranes that utilize functional materials to remove contaminants by adsorption or reaction simultaneously during filtration. Finally, we conclude with a discussion of regeneration strategies for sacrificial membranes and an outlook on opportunities and challenges in the field. The most promising regeneration strategies for removing spent layers and redepositing new ones are the in-situ procedures that align with the routine cleaning protocols widely adopted by the membrane industry.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"33 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991896","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}
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