The removal of antibiotics from pharmaceutical wastewater is of paramount importance from an environmental point of view. Although various techniques have been developed, it is still highly demanded to develop environmentally benign approaches that can make better use of chemicals in pharmaceutical wastewater for chemoenzymatic processes. Here we combine glucose oxidase (GOx) and hemin toward chemoenzymatic cascades for the degradation of tetracycline (TC) and the detection of phenol derivatives. Hemin was covalently attached to pre-crosslinked GOx aggregates through the Ugi four-component reaction, which could further crosslink the aggregates. The close proximity between GOx and hemin enables the rapid consumption of H2O2 generated from the oxidation of glucose. This consumption prevents the accumulation of H2O2 and in turn overcomes activity inhibition. The structure-activity relationship of hemin-modified crosslinked GOx aggregates (HCGOAs) was systematically investigated. They displayed excellent catalytic performance in the degradation of TC and the detection of phenol and bisphenol A. The HCGOAs are promising for pharmaceutical wastewater treatments.
{"title":"Hemin-modified crosslinked glucose oxidase aggregates for efficient degradation of tetracycline and detection of phenol derivatives","authors":"Xiaorong Xiong, Yizhuo Lu, Yan Peng, Meishuang Qiu, Tianyou Chen, Zushun Xu","doi":"10.1016/j.colsurfa.2025.136516","DOIUrl":"10.1016/j.colsurfa.2025.136516","url":null,"abstract":"<div><div>The removal of antibiotics from pharmaceutical wastewater is of paramount importance from an environmental point of view. Although various techniques have been developed, it is still highly demanded to develop environmentally benign approaches that can make better use of chemicals in pharmaceutical wastewater for chemoenzymatic processes. Here we combine glucose oxidase (GOx) and hemin toward chemoenzymatic cascades for the degradation of tetracycline (TC) and the detection of phenol derivatives. Hemin was covalently attached to pre-crosslinked GOx aggregates through the Ugi four-component reaction, which could further crosslink the aggregates. The close proximity between GOx and hemin enables the rapid consumption of H<sub>2</sub>O<sub>2</sub> generated from the oxidation of glucose. This consumption prevents the accumulation of H<sub>2</sub>O<sub>2</sub> and in turn overcomes activity inhibition. The structure-activity relationship of hemin-modified crosslinked GOx aggregates (HCGOAs) was systematically investigated. They displayed excellent catalytic performance in the degradation of TC and the detection of phenol and bisphenol A. The HCGOAs are promising for pharmaceutical wastewater treatments.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"713 ","pages":"Article 136516"},"PeriodicalIF":4.9,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143488624","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-25DOI: 10.1016/j.colsurfa.2025.136510
Yanxia Xie , Junjie Zhu , Liangyi Lv , Chunsheng Ai , Xinjian Zhu , Tianchen Zheng , Jie Yang , Hongjie Wang
Quartz yarn was widely used in glass fiber reinforced composites, while the defect derived from the poor permeability of resin solution in quartz yarn restricted its application. Although the permeability was widely studied and several test methods were proposed, the effect of the components of wetting agent on permeability was seldom reported, and an accurate method to characterized the permeability of fiber bundle needed to be explored. In this study, a new type of wetting agent was prepared to produce quartz yarn with high permeability by controlling the chemical components of the wetting agent, and the effects of them on permeability, wetting ability, bunching property, and mechanism were discussed, and a relatively accurate permeability method was proposed. The results showed the chemical components played a key role in affecting the permeability of quartz yarn. The wetting agent with low content of polar components (COP) and low content of solid content (COS) exhibited high permeability for quartz yarn, possessing better properties than commercial yarns. When the COP was high, the precipitated coupling agent lamellae on the surface of the yarn reduced the gap between the yarn fibers, resulting in a larger adhesive attachment rate and bunching property of the yarns. The mechanism of the action from the wetting agent components was analyzed by the FTIR spectrum, indicating that the COS and COP affected the fluidity and permeability of the resin between fibers. The study revealed the mechanism of chemical components of wetting on the permeability of quartz yarn and proposed a method to test the permeability of resin solution in quartz yarn. The results of this study provided experimental data and reference basis for the development of functional wetting agent.
{"title":"Preparation and study of quartz yarn with good permeability by controlling the content of polar components in wetting agent","authors":"Yanxia Xie , Junjie Zhu , Liangyi Lv , Chunsheng Ai , Xinjian Zhu , Tianchen Zheng , Jie Yang , Hongjie Wang","doi":"10.1016/j.colsurfa.2025.136510","DOIUrl":"10.1016/j.colsurfa.2025.136510","url":null,"abstract":"<div><div>Quartz yarn was widely used in glass fiber reinforced composites, while the defect derived from the poor permeability of resin solution in quartz yarn restricted its application. Although the permeability was widely studied and several test methods were proposed, the effect of the components of wetting agent on permeability was seldom reported, and an accurate method to characterized the permeability of fiber bundle needed to be explored. In this study, a new type of wetting agent was prepared to produce quartz yarn with high permeability by controlling the chemical components of the wetting agent, and the effects of them on permeability, wetting ability, bunching property, and mechanism were discussed, and a relatively accurate permeability method was proposed. The results showed the chemical components played a key role in affecting the permeability of quartz yarn. The wetting agent with low content of polar components (COP) and low content of solid content (COS) exhibited high permeability for quartz yarn, possessing better properties than commercial yarns. When the COP was high, the precipitated coupling agent lamellae on the surface of the yarn reduced the gap between the yarn fibers, resulting in a larger adhesive attachment rate and bunching property of the yarns. The mechanism of the action from the wetting agent components was analyzed by the FTIR spectrum, indicating that the COS and COP affected the fluidity and permeability of the resin between fibers. The study revealed the mechanism of chemical components of wetting on the permeability of quartz yarn and proposed a method to test the permeability of resin solution in quartz yarn. The results of this study provided experimental data and reference basis for the development of functional wetting agent.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"713 ","pages":"Article 136510"},"PeriodicalIF":4.9,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143488197","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Colloids in saturated porous media, such as soil and aquifers, play a critical role in the transport of nutrients, pollutants, and microorganisms. Their movement can influence the quality of groundwater and the effectiveness of filtration systems. Detecting colloids in these environments is essential for understanding contaminant spread, predicting soil and groundwater behavior, and managing water resources. Accurate detection helps in designing remediation strategies and ensures the safe use of natural resources, particularly in environmental engineering and hydrogeology. In this paper, we apply an artificial intelligence approach with the help of deep learning to detect colloids, which is a prerequisite for subsequent steps in porous media research. Since colloids are tiny particles and do not have enough information to identify, firstly we use an image processing technique called the dilation operation to improve distinguishing features of colloids for the detection process. This operation leads to achieving more accurate results for the detection of tiny colloids. Then, we propose a lightweight deep convolutional neural network to detect colloids automatically without the requirement for manual analysis. In our experiments, Precision, Recall, F-measure, and TCR metrics are employed for assessment. The experimental results show the efficiency and effectiveness of the proposed approach compared to six image processing methods in the detection process of colloids.
{"title":"An artificial intelligence image-based approach for colloid detection in saturated porous media","authors":"Behzad Mirzaei , Hossein Nezamabadi-pour , Amir Raoof , Reza Derakhshani","doi":"10.1016/j.colsurfa.2025.136503","DOIUrl":"10.1016/j.colsurfa.2025.136503","url":null,"abstract":"<div><div>Colloids in saturated porous media, such as soil and aquifers, play a critical role in the transport of nutrients, pollutants, and microorganisms. Their movement can influence the quality of groundwater and the effectiveness of filtration systems. Detecting colloids in these environments is essential for understanding contaminant spread, predicting soil and groundwater behavior, and managing water resources. Accurate detection helps in designing remediation strategies and ensures the safe use of natural resources, particularly in environmental engineering and hydrogeology. In this paper, we apply an artificial intelligence approach with the help of deep learning to detect colloids, which is a prerequisite for subsequent steps in porous media research. Since colloids are tiny particles and do not have enough information to identify, firstly we use an image processing technique called the dilation operation to improve distinguishing features of colloids for the detection process. This operation leads to achieving more accurate results for the detection of tiny colloids. Then, we propose a lightweight deep convolutional neural network to detect colloids automatically without the requirement for manual analysis. In our experiments, Precision, Recall, <em>F</em>-measure, and TCR metrics are employed for assessment. The experimental results show the efficiency and effectiveness of the proposed approach compared to six image processing methods in the detection process of colloids.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"713 ","pages":"Article 136503"},"PeriodicalIF":4.9,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518848","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-25DOI: 10.1016/j.colsurfa.2025.136506
Yuansheng Lin , Zhilong Guo , Suling Dong , Yixin Li , Bohong Kan , Kongyin Zhao , Sidi Li , Zhengchun Yang
Hydrogels showed superiorities in molecularly imprinting sensors for detecting biomolecules owing to their stimulus-responsive nature. However, the excessive swelling of hydrogel during the elution process damages the imprinting cavities, leading to a reduction in sensitivity. In this study, a molecularly imprinted electrochemical sensor was designed for rapid protein recognition. The sensor utilized a composite hydrogel based on hybrid cross-linked calcium alginate/calcium silicate (CaAlg/CaSiO3) to mitigate the excessive swelling of the CaAlg hydrogel. The preparation involved coating a bare carbon electrode with a sodium silicate-sodium alginate (Na2SiO3-NaAlg) mixed solution, cross-linking with CaCl2 solution, and eluting bovine serum albumin (BSA) with Tris-HCl solution. The incorporation of CaSiO3 nanoparticles stabilized the organic-inorganic hybrid structure, enhancing the hydrogel's resistance to swelling and maintaining cavity integrity. The molecularly imprinted polymer (MIP) sensor demonstrated high selectivity for BSA, excellent repeatability, long-term stability, and reproducibility, showing the potential for improved sensitivity in biomolecule detection.
{"title":"Protein imprinted CaAlg/CaSiO3 hybrid hydrogel modified electrochemical sensor for sensitive detection of BSA","authors":"Yuansheng Lin , Zhilong Guo , Suling Dong , Yixin Li , Bohong Kan , Kongyin Zhao , Sidi Li , Zhengchun Yang","doi":"10.1016/j.colsurfa.2025.136506","DOIUrl":"10.1016/j.colsurfa.2025.136506","url":null,"abstract":"<div><div>Hydrogels showed superiorities in molecularly imprinting sensors for detecting biomolecules owing to their stimulus-responsive nature. However, the excessive swelling of hydrogel during the elution process damages the imprinting cavities, leading to a reduction in sensitivity. In this study, a molecularly imprinted electrochemical sensor was designed for rapid protein recognition. The sensor utilized a composite hydrogel based on hybrid cross-linked calcium alginate/calcium silicate (CaAlg/CaSiO<sub>3</sub>) to mitigate the excessive swelling of the CaAlg hydrogel. The preparation involved coating a bare carbon electrode with a sodium silicate-sodium alginate (Na<sub>2</sub>SiO<sub>3</sub>-NaAlg) mixed solution, cross-linking with CaCl<sub>2</sub> solution, and eluting bovine serum albumin (BSA) with Tris-HCl solution. The incorporation of CaSiO<sub>3</sub> nanoparticles stabilized the organic-inorganic hybrid structure, enhancing the hydrogel's resistance to swelling and maintaining cavity integrity. The molecularly imprinted polymer (MIP) sensor demonstrated high selectivity for BSA, excellent repeatability, long-term stability, and reproducibility, showing the potential for improved sensitivity in biomolecule detection.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"713 ","pages":"Article 136506"},"PeriodicalIF":4.9,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143488194","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-25DOI: 10.1016/j.colsurfa.2025.136525
Yanhe Han , Hao Yao , Han Xu , Qingpeng Zhao , Nannan Wang , Shizong Wang , Xuejiao Ma
Molybdenum disulfide (MoS₂) has garnered significant attention as a highly efficient catalyst for hydrogen production due to its high activity, cost-effectiveness, and abundant availability. MoS2 has the disadvantages of poor electrical conductivity and slow electron transfer rate. Here in, a strategy of regulation of facet of MoS2 was developed to enhance the activity of MoS2 for hydrogen production. The results show that the incorporation of cerium dioxide (CeO2) and graphene oxide (GO) in MoS2 promoted the growth of MoS2 (002) and CeO2 (111) crystal surface, which increased the number of active sites and the surface area of the MoS2 electrode. In addition, the coupled facets of (002) of MoS2 and (111) of CeO2 reduced the intermediate energy barrier of the hydrolyzed ionization process for hydroxyl receptors, resulting in exceptional hydrogen evolution reaction (HER) performance and extended electrode lifespan. The TiO2/MoS2-CeO2/GO electrode achieved the current density of 10 mA/cm2 at an overpotential of 120 mV, a specific capacitance of 432.5 mF/cm2 and an AC impedance of 3.25Ω. The maximum hydrogen production and hydrogen production efficiency reached 24.54 mmol/(h·cm²) and 69.84 %, respectively, which are 1.53 times and 2.09 times higher than those of TiO2/MoS2 electrode, respectively. The Volmer-Heyrovsky mechanism for electrocatalytic hydrogen evolution was analyzed, and the stability and reusability of TiO2/MoS2-CeO2/GO electrode were confirmed through 3000 cycles of CV test and 20 h water electrolysis testing. Additionally, the effects of electrode material, input voltage, electrolyte concentration and electrolyte temperature on hydrogen production were investigated. The work provides reference for designing high-performance electrocatalytic hydrogen evolution electrode materials.
{"title":"Highly efficient CeO2/GO co-doped MoS2 catalyst for electrocatalytic hydrogen evolution performance","authors":"Yanhe Han , Hao Yao , Han Xu , Qingpeng Zhao , Nannan Wang , Shizong Wang , Xuejiao Ma","doi":"10.1016/j.colsurfa.2025.136525","DOIUrl":"10.1016/j.colsurfa.2025.136525","url":null,"abstract":"<div><div>Molybdenum disulfide (MoS₂) has garnered significant attention as a highly efficient catalyst for hydrogen production due to its high activity, cost-effectiveness, and abundant availability. MoS<sub>2</sub> has the disadvantages of poor electrical conductivity and slow electron transfer rate. Here in, a strategy of regulation of facet of MoS<sub>2</sub> was developed to enhance the activity of MoS<sub>2</sub> for hydrogen production. The results show that the incorporation of cerium dioxide (CeO<sub>2</sub>) and graphene oxide (GO) in MoS<sub>2</sub> promoted the growth of MoS<sub>2</sub> (002) and CeO<sub>2</sub> (111) crystal surface, which increased the number of active sites and the surface area of the MoS<sub>2</sub> electrode. In addition, the coupled facets of (002) of MoS<sub>2</sub> and (111) of CeO<sub>2</sub> reduced the intermediate energy barrier of the hydrolyzed ionization process for hydroxyl receptors, resulting in exceptional hydrogen evolution reaction (HER) performance and extended electrode lifespan. The TiO<sub>2</sub>/MoS<sub>2</sub>-CeO<sub>2</sub>/GO electrode achieved the current density of 10 mA/cm<sup>2</sup> at an overpotential of 120 mV, a specific capacitance of 432.5 mF/cm<sup>2</sup> and an AC impedance of 3.25Ω. The maximum hydrogen production and hydrogen production efficiency reached 24.54 mmol/(h·cm²) and 69.84 %, respectively, which are 1.53 times and 2.09 times higher than those of TiO<sub>2</sub>/MoS<sub>2</sub> electrode, respectively. The Volmer-Heyrovsky mechanism for electrocatalytic hydrogen evolution was analyzed, and the stability and reusability of TiO<sub>2</sub>/MoS<sub>2</sub>-CeO<sub>2</sub>/GO electrode were confirmed through 3000 cycles of CV test and 20 h water electrolysis testing. Additionally, the effects of electrode material, input voltage, electrolyte concentration and electrolyte temperature on hydrogen production were investigated. The work provides reference for designing high-performance electrocatalytic hydrogen evolution electrode materials.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"713 ","pages":"Article 136525"},"PeriodicalIF":4.9,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143511219","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-25DOI: 10.1016/j.colsurfa.2025.136507
Yaling Zhang , Guojun Cheng , Zhongfeng Tang , Qi Jin , Guoxin Ding , Xianglong Wan
Improving the thermal conductivity of the PVA film depends on the construction of efficient thermal conductivity network. However, the agglomeration and high thermal resistance of the nanoparticles limit the high thermal conductivity construction of the PVA-based films. The nano-SiO2 particles were modified using KH550 results in an even distribution, and then deposited onto the Ti3C2Tx MXene surfaces by electrostatic self-assembly. The dispersion and interaction of the modified SiO2/Ti3C2Tx MXene (mST) within the PVA matrix were investigated, and mST/PVA (mSTP) films were prepared in this job. The treatment of the mST fillers ensures uniform distribution and reduces interface resistance. The mechanical properties of the mSTP films were significantly improved, with the tensile strength and elongation at break increasing by 183 % and 115 %, respectively. The in-plane and out-plane thermal conductivity of the mSTP-7.5 film reached 2.11 W·m−1·K−1 and 0.58 W·m−1·K−1, respectively. The synergy between Ti3C2Tx MXene and nano-SiO2 forms a controllable cross-linking structure, greatly enhancing thermal and mechanical properties. It not only offer a practical technical approach but also provide new theoretical insights for the design and optimization of the thermally conductive composites.
{"title":"Excellent mechanical and thermal conductivity performance of polyvinyl alcohol film doped SiO2@Ti3C2Tx MXene via electrostatic nano-particle assembly","authors":"Yaling Zhang , Guojun Cheng , Zhongfeng Tang , Qi Jin , Guoxin Ding , Xianglong Wan","doi":"10.1016/j.colsurfa.2025.136507","DOIUrl":"10.1016/j.colsurfa.2025.136507","url":null,"abstract":"<div><div>Improving the thermal conductivity of the PVA film depends on the construction of efficient thermal conductivity network. However, the agglomeration and high thermal resistance of the nanoparticles limit the high thermal conductivity construction of the PVA-based films. The nano-SiO<sub>2</sub> particles were modified using KH550 results in an even distribution, and then deposited onto the Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> MXene surfaces by electrostatic self-assembly. The dispersion and interaction of the modified SiO<sub>2</sub>/Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> MXene (mST) within the PVA matrix were investigated, and mST/PVA (mSTP) films were prepared in this job. The treatment of the mST fillers ensures uniform distribution and reduces interface resistance. The mechanical properties of the mSTP films were significantly improved, with the tensile strength and elongation at break increasing by 183 % and 115 %, respectively. The in-plane and out-plane thermal conductivity of the mSTP-7.5 film reached 2.11 W·m<sup>−1</sup>·K<sup>−1</sup> and 0.58 W·m<sup>−1</sup>·K<sup>−1</sup>, respectively. The synergy between Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> MXene and nano-SiO<sub>2</sub> forms a controllable cross-linking structure, greatly enhancing thermal and mechanical properties. It not only offer a practical technical approach but also provide new theoretical insights for the design and optimization of the thermally conductive composites.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"713 ","pages":"Article 136507"},"PeriodicalIF":4.9,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143509344","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-25DOI: 10.1016/j.colsurfa.2025.136521
Fang Feng , Han Yin , Zijing Ren , Yang An , Firdoz Shaik , Bin Jiang
All-carbon electrodes are promising green bifunctional catalytic electrodes for cost-effective water splitting technology. Herein, we report on a series of N-based multi-heteroatom doped carbon quantum dots (CQDs) with varied concentrations that are placed on vertical graphene (VG) as bifunctional vinegar-derived all-carbon electrodes for total water splitting. A systematic analysis of the electrocatalytic performance of catalytic electrodes shows that N,S-VG-CQDs-0.8 exhibited enhanced hydrogen evolution reaction (overpotentials of 94 ± 10 mV and 97 ± 10 mV in acid and alkaline electrolytes, respectively) and oxygen evolution reaction (overpotentials of 305 ± 10 mV and 327 ± 10 mV in acid and alkaline electrolytes, respectively) performances. The unique strong synergistic impact of pyridine N and thiophene S, the increased concentration of CQDs, and the high electronegativity of the N and S atoms are all responsible for the improvement of N, S co-doped electrode performance, according to experimental findings and DFT calculations. In addition, the catalytic electrodes exhibit hydrogen evolution reaction (HER) stability (10 h) and Faraday efficiency (89.5 ± 2 %) in a wide pH range. This study provides significant information on the advancement and commercialization of high-performance all-carbon electrodes for water-splitting technology-based green hydrogen production.
{"title":"Vinegar-derived nitrogen-based multi-heteroatom doped bifunctional All-carbon electrodes for overall water splitting in a wide pH range","authors":"Fang Feng , Han Yin , Zijing Ren , Yang An , Firdoz Shaik , Bin Jiang","doi":"10.1016/j.colsurfa.2025.136521","DOIUrl":"10.1016/j.colsurfa.2025.136521","url":null,"abstract":"<div><div>All-carbon electrodes are promising green bifunctional catalytic electrodes for cost-effective water splitting technology. Herein, we report on a series of N-based multi-heteroatom doped carbon quantum dots (CQDs) with varied concentrations that are placed on vertical graphene (VG) as bifunctional vinegar-derived all-carbon electrodes for total water splitting. A systematic analysis of the electrocatalytic performance of catalytic electrodes shows that N,S-VG-CQDs-0.8 exhibited enhanced hydrogen evolution reaction (overpotentials of 94 ± 10 mV and 97 ± 10 mV in acid and alkaline electrolytes, respectively) and oxygen evolution reaction (overpotentials of 305 ± 10 mV and 327 ± 10 mV in acid and alkaline electrolytes, respectively) performances. The unique strong synergistic impact of pyridine N and thiophene S, the increased concentration of CQDs, and the high electronegativity of the N and S atoms are all responsible for the improvement of N, S co-doped electrode performance, according to experimental findings and DFT calculations. In addition, the catalytic electrodes exhibit hydrogen evolution reaction (HER) stability (10 h) and Faraday efficiency (89.5 ± 2 %) in a wide pH range. This study provides significant information on the advancement and commercialization of high-performance all-carbon electrodes for water-splitting technology-based green hydrogen production.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"713 ","pages":"Article 136521"},"PeriodicalIF":4.9,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143510134","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-25DOI: 10.1016/j.colsurfa.2025.136512
Xiaoming Zhang , Suli Wang , Zhangxun Xia , Huanqiao Li , Shansheng Yu , Gongquan Sun
Metal-nitrogen-carbon based single atom catalysts (SACs) have been the subject of oxygen reduction reaction (ORR) electrocatalysts for electrochemical devices. Nevertheless, the scaling relationship of ΔG*OOH, ΔG*OH and ΔG*O represents a significant obstacle to further enhancement of ORR efficiency for SACs. Accordingly, a confinement model X@M-N4/C electrocatalyst was constructed. The density functional theory calculations demonstrate that the overpotential of Br@Fe-N4/C54 (0.47 V vs. RHE) for ORR is significantly lower than that of Fe-N4/C54 (0.67 V vs. RHE). The variation in distance between the Br and Fe atoms during the ORR process provides evidence that supports the hypothesis that the Br atom regulates the Fe-N4 active center, through in-situ dynamic non-bonding coordination (dFe-Br>3 Å). The confined Br atom results in an increase in ΔG*OH and a decrease in ΔG*O. This results in a disruption of the linear relationship and a reduction in the overpotential associated with the rate-determining elementary reaction (*O+H++e-→*OH). The Fe-N4 active center facilitates the sequential ORR catalytic process through in-situ dynamic regulation of the trapped Br atom. This conclusion is also applicable to Br@Fe-N4/graphene and Br@Fe-N4/CNT. The findings of our research represent a significant advancement in the field of enhancing the performance of SACs for multi-electron electrocatalytic reactions.
{"title":"The dynamic regulation effect in X@Fe-N4/C electrocatalyst for the sequential oxygen reduction reaction","authors":"Xiaoming Zhang , Suli Wang , Zhangxun Xia , Huanqiao Li , Shansheng Yu , Gongquan Sun","doi":"10.1016/j.colsurfa.2025.136512","DOIUrl":"10.1016/j.colsurfa.2025.136512","url":null,"abstract":"<div><div>Metal-nitrogen-carbon based single atom catalysts (SACs) have been the subject of oxygen reduction reaction (ORR) electrocatalysts for electrochemical devices. Nevertheless, the scaling relationship of ΔG<sub>*OOH</sub>, ΔG<sub>*OH</sub> and ΔG<sub>*O</sub> represents a significant obstacle to further enhancement of ORR efficiency for SACs. Accordingly, a confinement model X@M-N<sub>4</sub>/C electrocatalyst was constructed. The density functional theory calculations demonstrate that the overpotential of Br@Fe-N<sub>4</sub>/C54 (0.47 V <em>vs.</em> RHE) for ORR is significantly lower than that of Fe-N<sub>4</sub>/C54 (0.67 V <em>vs.</em> RHE). The variation in distance between the Br and Fe atoms during the ORR process provides evidence that supports the hypothesis that the Br atom regulates the Fe-N<sub>4</sub> active center, through in-situ dynamic non-bonding coordination (<em>d</em><sub><em>Fe-Br</em></sub>>3 Å). The confined Br atom results in an increase in ΔG<sub>*OH</sub> and a decrease in ΔG<sub>*O</sub>. This results in a disruption of the linear relationship and a reduction in the overpotential associated with the rate-determining elementary reaction (*O+H<sup>+</sup>+e<sup>-</sup>→*OH). The Fe-N<sub>4</sub> active center facilitates the sequential ORR catalytic process through in-situ dynamic regulation of the trapped Br atom. This conclusion is also applicable to Br@Fe-N<sub>4</sub>/graphene and Br@Fe-N<sub>4</sub>/CNT. The findings of our research represent a significant advancement in the field of enhancing the performance of SACs for multi-electron electrocatalytic reactions.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"713 ","pages":"Article 136512"},"PeriodicalIF":4.9,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143511110","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-25DOI: 10.1016/j.colsurfa.2025.136524
Zhang Yongjia , Md. Amirul Islam , Bidyut Baran Saha
A metal-organic framework (MOF) is a crystalline material that exhibits distinctive physical and chemical properties due to the coordination between metal ions and organic ligands. These properties, including a high surface area, adjustable porosity, and the ability to easily modify the chemical composition, collectively render MOFs advantageous for adsorption and separation applications. Introducing polar groups and bimetallic components into the MOF structure could significantly enhance CO2 adsorption performance. This article investigated the impact of integrating these two approaches on CO2 capture. Three Lewis acid metal ions (Al3+, Fe3+, and Cu2+) were doped into MOFs, specifically UiO-66 and UiO-66-NH2. A range of characterization techniques were employed to facilitate comparison and verification of the results, including N2 adsorption, powder X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, and thermogravimetric analysis. This study then evaluated CO2 adsorption at varying temperatures. The findings indicated that the Fe3+-doped samples exhibited the best performance irrespective of the presence of amino groups. Notably, the higher the concentration of metal dopants in UiO-66, the greater the adsorption capacity. UiO-66(Zr1 Fe1) exhibited the highest CO2 adsorption capacity of 2.22 mmol per gram of the modified MOF. In contrast, modified UiO-66-NH2 exhibited the opposite trend, where the lower the metal doping level, the higher the adsorption capacity. UiO-66-NH2(Zr5 Fe1) exhibited the highest adsorption capacity of 3.5 mmol/g.
{"title":"Experimental investigation of CO₂ adsorption capacities in bimetallic-doped UiO-66 and UiO-66-NH2 frameworks","authors":"Zhang Yongjia , Md. Amirul Islam , Bidyut Baran Saha","doi":"10.1016/j.colsurfa.2025.136524","DOIUrl":"10.1016/j.colsurfa.2025.136524","url":null,"abstract":"<div><div>A metal-organic framework (MOF) is a crystalline material that exhibits distinctive physical and chemical properties due to the coordination between metal ions and organic ligands. These properties, including a high surface area, adjustable porosity, and the ability to easily modify the chemical composition, collectively render MOFs advantageous for adsorption and separation applications. Introducing polar groups and bimetallic components into the MOF structure could significantly enhance CO<sub>2</sub> adsorption performance. This article investigated the impact of integrating these two approaches on CO<sub>2</sub> capture. Three Lewis acid metal ions (Al<sup>3</sup><sup>+</sup>, Fe<sup>3+</sup>, and Cu<sup>2+</sup>) were doped into MOFs, specifically UiO-66 and UiO-66-NH<sub>2</sub>. A range of characterization techniques were employed to facilitate comparison and verification of the results, including N<sub>2</sub> adsorption, powder X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, and thermogravimetric analysis. This study then evaluated CO<sub>2</sub> adsorption at varying temperatures. The findings indicated that the Fe<sup>3+</sup>-doped samples exhibited the best performance irrespective of the presence of amino groups. Notably, the higher the concentration of metal dopants in UiO-66, the greater the adsorption capacity. UiO-66(Zr<sub>1</sub> Fe<sub>1</sub>) exhibited the highest CO<sub>2</sub> adsorption capacity of 2.22 mmol per gram of the modified MOF. In contrast, modified UiO-66-NH<sub>2</sub> exhibited the opposite trend, where the lower the metal doping level, the higher the adsorption capacity. UiO-66-NH<sub>2</sub>(Zr<sub>5</sub> Fe<sub>1</sub>) exhibited the highest adsorption capacity of 3.5 mmol/g.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"713 ","pages":"Article 136524"},"PeriodicalIF":4.9,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518992","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-25DOI: 10.1016/j.colsurfa.2025.136509
Haojie Xu , Junfeng Wang , Yuanping Huo , Ziwen Zuo , Jiang Yao , Wei Zhang
Sessile droplet evaporation under an electric field has become a promising cooling solution for high-power electronics, and the complicated heat transfer enhancement mechanism attracts much research attention. This study numerically investigated the effects of corona wind on the evaporation of sessile droplets. A needle-to-plate electrode configuration was employed, where the needle electrode was applied with high potential while the plate electrode was grounded. The relationships between the discharge properties, corona wind characteristics, droplet morphology evolution, internal Marangoni flow, temperature distribution, and vapor concentration were discussed. The results demonstrate that the accelerated ionized particles would generate an airflow from the needle electrode to the plate electrode, of which the maximum velocity was approximately 6.81 m/s with a + 20 kV applied electric potential. As a result, the lifetime of the evaporating droplets was found to significantly decrease from 228 s to 55 s. The internal Marangoni flow was strengthened by corona wind due to the interfacial cooling effects, whereas the shearing effects were rather negligible. In addition, the evaporating droplets with corona wind were likely to show a lower temperature than the neutral conditions, and the temperature distribution was highly dependent on the Marangoni flow pattern. In contrast, the shearing effects of corona wind would significantly increase the vapor concentration gradient, resulting in an improved evaporation rate. Finally, the local heat flux from hot substrates to the evaporating droplets was reported to be enhanced by the corona wind but with a low energy conversion efficiency of about 4.4 %. This work delivers crucial perspectives on the enhancement of sessile droplet evaporation.
{"title":"Numerical simulation of sessile droplet evaporation enhanced by corona wind","authors":"Haojie Xu , Junfeng Wang , Yuanping Huo , Ziwen Zuo , Jiang Yao , Wei Zhang","doi":"10.1016/j.colsurfa.2025.136509","DOIUrl":"10.1016/j.colsurfa.2025.136509","url":null,"abstract":"<div><div>Sessile droplet evaporation under an electric field has become a promising cooling solution for high-power electronics, and the complicated heat transfer enhancement mechanism attracts much research attention. This study numerically investigated the effects of corona wind on the evaporation of sessile droplets. A needle-to-plate electrode configuration was employed, where the needle electrode was applied with high potential while the plate electrode was grounded. The relationships between the discharge properties, corona wind characteristics, droplet morphology evolution, internal Marangoni flow, temperature distribution, and vapor concentration were discussed. The results demonstrate that the accelerated ionized particles would generate an airflow from the needle electrode to the plate electrode, of which the maximum velocity was approximately 6.81 m/s with a + 20 kV applied electric potential. As a result, the lifetime of the evaporating droplets was found to significantly decrease from 228 s to 55 s. The internal Marangoni flow was strengthened by corona wind due to the interfacial cooling effects, whereas the shearing effects were rather negligible. In addition, the evaporating droplets with corona wind were likely to show a lower temperature than the neutral conditions, and the temperature distribution was highly dependent on the Marangoni flow pattern. In contrast, the shearing effects of corona wind would significantly increase the vapor concentration gradient, resulting in an improved evaporation rate. Finally, the local heat flux from hot substrates to the evaporating droplets was reported to be enhanced by the corona wind but with a low energy conversion efficiency of about 4.4 %. This work delivers crucial perspectives on the enhancement of sessile droplet evaporation.</div></div>","PeriodicalId":278,"journal":{"name":"Colloids and Surfaces A: Physicochemical and Engineering Aspects","volume":"713 ","pages":"Article 136509"},"PeriodicalIF":4.9,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143510132","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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