Pub Date : 2024-11-07DOI: 10.1016/j.ces.2024.120913
Jianguo Zhuang , Yingjie Guan , Bihong Li , Haidan Wu , Jisheng Yu , Siyan Yan , Zhaojie Su , Tianyun Wang , Xuedong Zhu , Fan Yang
Anchoring active metal particles in zeolite cages can significantly improve catalytic stability. In this study, hollow silicalite-1 (HoS-1) encapsulated Ni nanoparticles catalyst (Ni@HoS-1) was prepared using the impregnation method and applied in MA hydrogenation. The encapsulation mechanism was explained as the zeolite wall restricting the evaporation of water in HoS-1, hence Ni particles would be spontaneously enriched within the zeolite cage after drying and calcination. Experiments revealed the specially designed structure effectively protected Ni particles from leaching, and after 5 cycles in liquid-phase batch reactions, the final MA conversion of Ni@HoS-1 is 40.8 % higher than that of Ni/S-1 (85.5 % vs 44.7 %). Moreover, the low acidity of Ni@HoS-1 also delayed the accumulation of carbon deposits, extending the continuous reaction lifespan from 128 h of Ni/S-1 to 188 h. These findings provided a new perspective for the controllable locating of active metal sites against the supports.
{"title":"Hollow silicalite-1 encapsulated nickel nanoparticles as highly stable catalysts in maleic anhydride hydrogenation","authors":"Jianguo Zhuang , Yingjie Guan , Bihong Li , Haidan Wu , Jisheng Yu , Siyan Yan , Zhaojie Su , Tianyun Wang , Xuedong Zhu , Fan Yang","doi":"10.1016/j.ces.2024.120913","DOIUrl":"10.1016/j.ces.2024.120913","url":null,"abstract":"<div><div>Anchoring active metal particles in zeolite cages can significantly improve catalytic stability. In this study, hollow silicalite-1 (HoS-1) encapsulated Ni nanoparticles catalyst (Ni@HoS-1) was prepared using the impregnation method and applied in MA hydrogenation. The encapsulation mechanism was explained as the zeolite wall restricting the evaporation of water in HoS-1, hence Ni particles would be spontaneously enriched within the zeolite cage after drying and calcination. Experiments revealed the specially designed structure effectively protected Ni particles from leaching, and after 5 cycles in liquid-phase batch reactions, the final MA conversion of Ni@HoS-1 is 40.8 % higher than that of Ni/S-1 (85.5 % <em>vs</em> 44.7 %). Moreover, the low acidity of Ni@HoS-1 also delayed the accumulation of carbon deposits, extending the continuous reaction lifespan from 128 h of Ni/S-1 to 188 h. These findings provided a new perspective for the controllable locating of active metal sites against the supports.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"302 ","pages":"Article 120913"},"PeriodicalIF":4.1,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594481","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A green synthesis route of ordered mesoporous carbon by nanocasting of sucrose/sodium metasilicate with template removal only by hot water (70 °C) is proposed. The metasilicate-sucrose mesoporous carbon (MSMC) was characterized by structural, textural, surface chemistry properties and their effect on ciprofloxacin (CIP) adsorption. Phenomenological modeling was applied, including two surface-reaction models: adsorption on adsorbent sites (AAS) and on heterogeneous surface (AHS), and two mass transfer models: external film (EFD) and intraparticle homogeneous (IHD) diffusion. A controlled porous structure containing mesopores (3.8 nm) with micropores (1.8 and 0.87 nm) allowed the “pore filling effect” mechanism and strongly favorable kinetics. A highly oxygenated carbon material (C: 81.84% O: 15.04% Si: 1.72% Na: 1.29%) with efficient template removal was obtained. Unusual behavior of the rate-limiting step (AAS or IHD) as a function of CIP concentrations was observed, with mechanism changes due to self-aggregation of CIP molecules (dimers, trimers and tetramers).
{"title":"Eco-friendly micro-mesoporous carbon from sucrose and sodium metasilicate template for ciprofloxacin adsorption: Effect of molecules self-association over diffusion mechanisms","authors":"Carla Santolin , Kêissedy Veridiane Hübner , Ricardo Schneider , Helton José Alves , Nader Marzban , Fabiano Bisinella Scheufele","doi":"10.1016/j.ces.2024.120907","DOIUrl":"10.1016/j.ces.2024.120907","url":null,"abstract":"<div><div>A green synthesis route of ordered mesoporous carbon by nanocasting of sucrose/sodium metasilicate with template removal only by hot water (70 °C) is proposed. The metasilicate-sucrose mesoporous carbon (MSMC) was characterized by structural, textural, surface chemistry properties and their effect on ciprofloxacin (CIP) adsorption. Phenomenological modeling was applied, including two surface-reaction models: adsorption on adsorbent sites (AAS) and on heterogeneous surface (AHS), and two mass transfer models: external film (EFD) and intraparticle homogeneous (IHD) diffusion. A controlled porous structure containing mesopores (3.8 nm) with micropores (1.8 and 0.87 nm) allowed the “pore filling effect” mechanism and strongly favorable kinetics. A highly oxygenated carbon material (C: 81.84% O: 15.04% Si: 1.72% Na: 1.29%) with efficient template removal was obtained. Unusual behavior of the rate-limiting step (AAS or IHD) as a function of CIP concentrations was observed, with mechanism changes due to self-aggregation of CIP molecules (dimers, trimers and tetramers).</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"302 ","pages":"Article 120907"},"PeriodicalIF":4.1,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594572","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-07DOI: 10.1016/j.ces.2024.120908
Zhixuan Tan , Xiaoyao Fan , Qiqi Fan , Siqi Lu , Tian Yu , Lihang Ma , Yuxuan Luo , Jing Li , Hao Li , Yi-bo Hu
Recovery of phosphate (PO4-P) from the aqueous environment is crucial for sustainable eutrophication and phosphorus resource management. In this study, aluminum hydroxide-coated nanoscale zero-valent iron (NZVI@Al(OH)3) was developed as a magnetic-recyclable, air-stable, and efficient adsorbent for aqueous PO4-P removal and recovery. The Al(OH)3 shell could effectively protect the NZVI core from corrosion by O2 and H+ under aerobic and anaerobic conditions, keeping the NZVI@Al(OH)3 magnetically recyclable after adsorption. In addition, the Al(OH)3 shell adsorbs PO4-P efficiently via Al-O-P inner-sphere complexation, which was not affected by atmospheric conditions, pH conditions, and the co-existing anions and natural organic matter in real surface waters. After adsorption, PO4-P can be readily desorbed by facile immersion of used NZVI@Al(OH)3 in a highly alkaline solution and precipitated as hydroxylapatitle, with bare NZVI and dissolved AlO2- recovered for recycling. Therefore, NZVI@Al(OH)3 is a robust and cost-effective adsorbent for PO4-P recovery under real surface water conditions.
{"title":"Phosphate recovery from aqueous environment with recyclable nanoscale zero-valent iron coated with aluminum hydroxide","authors":"Zhixuan Tan , Xiaoyao Fan , Qiqi Fan , Siqi Lu , Tian Yu , Lihang Ma , Yuxuan Luo , Jing Li , Hao Li , Yi-bo Hu","doi":"10.1016/j.ces.2024.120908","DOIUrl":"10.1016/j.ces.2024.120908","url":null,"abstract":"<div><div>Recovery of phosphate (PO<sub>4</sub>-P) from the aqueous environment is crucial for sustainable eutrophication and phosphorus resource management. In this study, aluminum hydroxide-coated nanoscale zero-valent iron (NZVI@Al(OH)<sub>3</sub>) was developed as a magnetic-recyclable, air-stable, and efficient adsorbent for aqueous PO<sub>4</sub>-P removal and recovery. The Al(OH)<sub>3</sub> shell could effectively protect the NZVI core from corrosion by O<sub>2</sub> and H<sup>+</sup> under aerobic and anaerobic conditions, keeping the NZVI@Al(OH)<sub>3</sub> magnetically recyclable after adsorption. In addition, the Al(OH)<sub>3</sub> shell adsorbs PO<sub>4</sub>-P efficiently via Al-O-P inner-sphere complexation, which was not affected by atmospheric conditions, pH conditions, and the co-existing anions and natural organic matter in real surface waters. After adsorption, PO<sub>4</sub>-P can be readily desorbed by facile immersion of used NZVI@Al(OH)<sub>3</sub> in a highly alkaline solution and precipitated as hydroxylapatitle, with bare NZVI and dissolved AlO<sub>2</sub><sup>-</sup> recovered for recycling. Therefore, NZVI@Al(OH)<sub>3</sub> is a robust and cost-effective adsorbent for PO<sub>4</sub>-P recovery under real surface water conditions.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"302 ","pages":"Article 120908"},"PeriodicalIF":4.1,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599277","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-07DOI: 10.1016/j.ces.2024.120910
Zilong Li , Nuo Xu , Shihua Liu , Yawen Wang , Vishnu D. Rajput , Tatiana Minkina , Faying Fan , Wa Gao , Yufei Zhao
The automotive, electronics, and aerospace sectors use electroless nickel plating (ENP) technology for surface treatment. Hypophosphite, a widely used reducing agent in ENP, generates large volumes of hypophosphate (H2PO2-) and nickel ions (Ni2+) in its wastewater which poses potential risks to human health. However, it is a highly challenging task to remove and recycle the H2PO2- and Ni2+ from such wastewater. In this study, a novel electrocatalysis coupled super-stable mineralization process was developed for the treatment of phosphorus-containing ENP wastewater. The electrocatalytic system, utilizing commercial lead dioxide and stainless steel as the anode and cathode, separately, achieved remarkable results in simultaneously removing H2PO2- and recycling valuable Ni2+ ions from ENP wastewater, with a 99.1 % oxidation efficiency for H2PO2- to PO43- and a high recovery rate of 99.8 % for nickel. In order to meet industrial emission standards, layered double hydroxide (CaAl-LDH) and its calcined derivatives (CaAl-900) were employed as super-stable mineralizers for the further treatment of total phosphorus (TP) and residual Ni2+ in the wastewater. The mechanism underlying the enhanced treatment of ENP wastewater was elucidated through free radical quenching experiments, revealed superoxide radicals (·O2–) as the primary active species. It is noteworthy that the successful treatment of actual ENP wastewater was achieved, meeting standard discharge requirements. This study provides novel insights for achieving resource-efficient wastewater treatment and promoting environmentally friendly electroplating industries.
{"title":"Electrocatalysis coupled super-stable mineralization for the efficient treatment of phosphorus containing plating wastewater","authors":"Zilong Li , Nuo Xu , Shihua Liu , Yawen Wang , Vishnu D. Rajput , Tatiana Minkina , Faying Fan , Wa Gao , Yufei Zhao","doi":"10.1016/j.ces.2024.120910","DOIUrl":"10.1016/j.ces.2024.120910","url":null,"abstract":"<div><div>The automotive, electronics, and aerospace sectors use electroless nickel plating (ENP) technology for surface treatment. Hypophosphite, a widely used reducing agent in ENP, generates large volumes of hypophosphate (H<sub>2</sub>PO<sub>2</sub><sup>-</sup>) and nickel ions (Ni<sup>2+</sup>) in its wastewater which poses potential risks to human health. However, it is a highly challenging task to remove and recycle the H<sub>2</sub>PO<sub>2</sub><sup>-</sup> and Ni<sup>2+</sup> from such wastewater. In this study, a novel electrocatalysis coupled super-stable mineralization process was developed for the treatment of phosphorus-containing ENP wastewater. The electrocatalytic system, utilizing commercial lead dioxide and stainless steel as the anode and cathode, separately, achieved remarkable results in simultaneously removing H<sub>2</sub>PO<sub>2</sub><sup>-</sup> and recycling valuable Ni<sup>2+</sup> ions from ENP wastewater, with a 99.1 % oxidation efficiency for H<sub>2</sub>PO<sub>2</sub><sup>-</sup> to PO<sub>4</sub><sup>3-</sup> and a high recovery rate of 99.8 % for nickel. In order to meet industrial emission standards, layered double hydroxide (CaAl-LDH) and its calcined derivatives (CaAl-900) were employed as super-stable mineralizers for the further treatment of total phosphorus (TP) and residual Ni<sup>2+</sup> in the wastewater. The mechanism underlying the enhanced treatment of ENP wastewater was elucidated through free radical quenching experiments, revealed superoxide radicals (·O<sub>2</sub><sup>–</sup>) as the primary active species. It is noteworthy that the successful treatment of actual ENP wastewater was achieved, meeting standard discharge requirements. This study provides novel insights for achieving resource-efficient wastewater treatment and promoting environmentally friendly electroplating industries.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"302 ","pages":"Article 120910"},"PeriodicalIF":4.1,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594480","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-07DOI: 10.1016/j.ces.2024.120916
Song He , Wenli Du , Xin Peng , Xin Li
Material synthesis literature documents detailed synthesis procedures, which provide valuable insight and guidance for designing practical synthesis routes. Information extraction (IE) techniques have emerged as powerful tools to obtain structured synthesis-related data. However, current IE methods struggle to differentiate semantically similar experimental records and extract dense experimental properties with abstract expressions, limiting their effectiveness in the zeolite synthesis domain. To this end, we propose ZeoReader, an end-to-end IE framework designed to extract synthesis steps from zeolite synthesis literature. Specifically, to effectively distinguish between semantically similar descriptions of synthesis and characterization experiments, ZeoReader constructs a MatSciBERT-based paragraph classifier that offers rich prior synthesis knowledge. For improving the extraction of complete synthesis steps in complex sentences, ZeoReader develops a two-stage synthesis step extraction model, which introduces customized contrastive learning to model the distributions of dense properties and capture features of abstract expressions. Furthermore, domain-specific parsing strategies are proposed to enable ZeoReader to automatically parse PDF documents, identify synthesis experimental passages, and extract structured zeolite synthesis steps containing actions and corresponding experimental properties. Extensive experiments demonstrate that ZeoReader detects synthesis passages with an accuracy of 94.06% on out-of-sample documents and extracts experimental actions and properties with an F1 score of 93.05% and 74.99%, respectively. Our proposed IE framework can be embedded in autonomous unmanned zeolite synthesis experiments to rapidly understand, reproduce and validate existing experimental routes, thus facilitating new zeolite exploration.
{"title":"ZeoReader: Automated extraction of synthesis steps from zeolite synthesis literature for autonomous experiments","authors":"Song He , Wenli Du , Xin Peng , Xin Li","doi":"10.1016/j.ces.2024.120916","DOIUrl":"10.1016/j.ces.2024.120916","url":null,"abstract":"<div><div>Material synthesis literature documents detailed synthesis procedures, which provide valuable insight and guidance for designing practical synthesis routes. Information extraction (IE) techniques have emerged as powerful tools to obtain structured synthesis-related data. However, current IE methods struggle to differentiate semantically similar experimental records and extract dense experimental properties with abstract expressions, limiting their effectiveness in the zeolite synthesis domain. To this end, we propose ZeoReader, an end-to-end IE framework designed to extract synthesis steps from zeolite synthesis literature. Specifically, to effectively distinguish between semantically similar descriptions of synthesis and characterization experiments, ZeoReader constructs a MatSciBERT-based paragraph classifier that offers rich prior synthesis knowledge. For improving the extraction of complete synthesis steps in complex sentences, ZeoReader develops a two-stage synthesis step extraction model, which introduces customized contrastive learning to model the distributions of dense properties and capture features of abstract expressions. Furthermore, domain-specific parsing strategies are proposed to enable ZeoReader to automatically parse PDF documents, identify synthesis experimental passages, and extract structured zeolite synthesis steps containing actions and corresponding experimental properties. Extensive experiments demonstrate that ZeoReader detects synthesis passages with an accuracy of 94.06% on out-of-sample documents and extracts experimental actions and properties with an F1 score of 93.05% and 74.99%, respectively. Our proposed IE framework can be embedded in autonomous unmanned zeolite synthesis experiments to rapidly understand, reproduce and validate existing experimental routes, thus facilitating new zeolite exploration.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"302 ","pages":"Article 120916"},"PeriodicalIF":4.1,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594482","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-07DOI: 10.1016/j.ces.2024.120906
Premchand Premchand , Shannon Mead , Debora Fino , Francesca Demichelis , Samir Bensaid , David Chiaramonti , Elsa Antunes
In this study, cigarette butts (CB) waste was pyrolyzed over a wide temperature range (400–700 °C) using Pyro/GC–MS and slow pyrolysis experiments. The feedstock and char products were extensively investigated using TGA, elemental analysis, surface area and porosity analysis, SEM-EDS, XRD, and FT-IR, and subsequently tested for their ability to remove Ni (II) and Cu (II) from aqueous solutions. The Pyro/GC–MS analysis revealed the presence of several useful compounds including acids, esters and hydrocarbons. Char yields ranged from 26.6 to 20.1 wt%, and carbon contents varied from 65.3 to 60.8 wt%. The chars produced at medium temperatures (500-600 °C) were highly porous, with a specific surface area of 272.9–270.8 m2/g. The heavy metal adsorption studies revealed that CB 500 °C had the highest adsorption capacity of 13.8 mg/g with 53.4 % nickel removal, while CB 600 °C had the highest adsorption capacity of 23.4 mg/g with 94.7 % copper removal.
在这项研究中，利用 Pyro/GC-MS 和缓慢热解实验，在较宽的温度范围（400-700 °C）内对烟蒂（CB）废料进行了热解。使用 TGA、元素分析、表面积和孔隙率分析、SEM-EDS、XRD 和 FT-IR 对原料和焦炭产品进行了广泛研究，随后测试了它们从水溶液中去除 Ni (II) 和 Cu (II) 的能力。Pyro/GC-MS 分析表明，其中存在多种有用的化合物，包括酸、酯和碳氢化合物。炭产量从 26.6% 到 20.1%不等，碳含量从 65.3% 到 60.8%不等。在中温（500-600 °C）下生产的炭具有高多孔性，比表面积为 272.9-270.8 m2/g。重金属吸附研究表明，CB 500 °C 的吸附容量最高，为 13.8 mg/g，镍去除率为 53.4%；CB 600 °C 的吸附容量最高，为 23.4 mg/g，铜去除率为 94.7%。
{"title":"Sustainable valorisation of cigarette butts waste through pyrolysis: An insight into the pyrolytic products and subsequent aqueous heavy metals removal by pyrolytic char","authors":"Premchand Premchand , Shannon Mead , Debora Fino , Francesca Demichelis , Samir Bensaid , David Chiaramonti , Elsa Antunes","doi":"10.1016/j.ces.2024.120906","DOIUrl":"10.1016/j.ces.2024.120906","url":null,"abstract":"<div><div>In this study, cigarette butts (CB) waste was pyrolyzed over a wide temperature range (400–700 °C) using Pyro/GC–MS and slow pyrolysis experiments. The feedstock and char products were extensively investigated using TGA, elemental analysis, surface area and porosity analysis, SEM-EDS, XRD, and FT-IR, and subsequently tested for their ability to remove Ni (II) and Cu (II) from aqueous solutions. The Pyro/GC–MS analysis revealed the presence of several useful compounds including acids, esters and hydrocarbons. Char yields ranged from 26.6 to 20.1 wt%, and carbon contents varied from 65.3 to 60.8 wt%. The chars produced at medium temperatures (500-600 °C) were highly porous, with a specific surface area of 272.9–270.8 m<sup>2</sup>/g. The heavy metal adsorption studies revealed that CB 500 °C had the highest adsorption capacity of 13.8 mg/g with 53.4 % nickel removal, while CB 600 °C had the highest adsorption capacity of 23.4 mg/g with 94.7 % copper removal.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"302 ","pages":"Article 120906"},"PeriodicalIF":4.1,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594176","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-06DOI: 10.1016/j.ces.2024.120900
Hardy Shuwanto , Jenni Lie , Hairus Abdullah , Subur P. Pasaribu , Indra Masmur
In this study, ZnIn2S4 with oxygen vacancies was fabricated using NaBH4-assisted hydrothermal method to enhance the photocatalytic activities. The generated ZIS and ZISVo-x samples exhibited microspherical nanosheet structure and it is proven that NaBH4 could enhance the amount of oxygen vacancies in ZnIn2S4 as confirmed by XPS analysis. Upon solar light irradiation, ZISVo-5 sample performed a fast photodegradation of tetracycline (TC) within 10 min and simultaneously exhibited a hydrogen evolution amount of ∼ 12 mmol (AQE = 6.07 at 420 nm), which is 2.75 times higher than that of pristine ZnIn2S4 (4.4 mmol). The degraded products of TC were further identified using LC-MS. The excellent photocatalytic HER performance was attributed to the optimum amount of oxygen vacancies in ZISVo-5 sample and the reactive oxygen species of •OH, O2•-, and 1O2 as confirmed by ESR analysis under light irradiation played a vital role for the rapid degradation of TC by ZISVo-5.
{"title":"Boosting photocatalytic hydrogen generation and Photo-Destruction of Tetracycline by In-Situ oxygen vacancies ZnIn2S4","authors":"Hardy Shuwanto , Jenni Lie , Hairus Abdullah , Subur P. Pasaribu , Indra Masmur","doi":"10.1016/j.ces.2024.120900","DOIUrl":"10.1016/j.ces.2024.120900","url":null,"abstract":"<div><div>In this study, ZnIn<sub>2</sub>S<sub>4</sub> with oxygen vacancies was fabricated using NaBH<sub>4</sub>-assisted hydrothermal method to enhance the photocatalytic activities. The generated ZIS and ZISVo-x samples exhibited microspherical nanosheet structure and it is proven that NaBH<sub>4</sub> could enhance the amount of oxygen vacancies in ZnIn<sub>2</sub>S<sub>4</sub> as confirmed by XPS analysis. Upon solar light irradiation, ZISVo-5 sample performed a fast photodegradation of tetracycline (TC) within 10 min and simultaneously exhibited a hydrogen evolution amount of ∼ 12 mmol (AQE = 6.07 at 420 nm), which is 2.75 times higher than that of pristine ZnIn<sub>2</sub>S<sub>4</sub> (4.4 mmol). The degraded products of TC were further identified using LC-MS. The excellent photocatalytic HER performance was attributed to the optimum amount of oxygen vacancies in ZISVo-5 sample and the reactive oxygen species of •OH, O<sub>2</sub><sup>•-</sup>, and <sup>1</sup>O<sub>2</sub> as confirmed by ESR analysis under light irradiation played a vital role for the rapid degradation of TC by ZISVo-5.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"302 ","pages":"Article 120900"},"PeriodicalIF":4.1,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588412","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-06DOI: 10.1016/j.ces.2024.120915
Hongbo Zhao , Jichao Zhu , Junfeng Wang , Lifang Hu
In this work, rice husk-derived hierarchical porous carbon (HPC) was developed as a high-performance adsorbent for ethyl mercaptan removal. Various characterization methods were used to comprehensively characterize the HPC adsorbent. HPC-2 exhibited an adsorption capacity of 118.1 mg/g for ethyl mercaptan at 500 ppm and a space velocity of 12000 h−1, outperforming similar materials reported previously. The high adsorption capacity was attributed to the material’s well-developed microporosity and the abundance of hydroxyl groups (–OH) on its surface, facilitating the chemisorption of ethyl mercaptan. Given the chemically adsorbed nature of sulfur compounds, N2 thermal regeneration was insufficient to fully recover the adsorbent’s performance. However, oxidative regeneration using O2/N2 (3/97 v/v) at 250 °C successfully removed these compounds and restored desulfurization efficiency, likely due to oxygen-assisted reactions on the adsorbent surface. This study provides valuable insights for effectively treating sulfur-containing odorous gases in the air.
{"title":"Highly efficient adsorption of ethyl mercaptan on hierarchical porous carbon derived from rice husk","authors":"Hongbo Zhao , Jichao Zhu , Junfeng Wang , Lifang Hu","doi":"10.1016/j.ces.2024.120915","DOIUrl":"10.1016/j.ces.2024.120915","url":null,"abstract":"<div><div>In this work, rice husk-derived hierarchical porous carbon (HPC) was developed as a high-performance adsorbent for ethyl mercaptan removal. Various characterization methods were used to comprehensively characterize the HPC adsorbent. HPC-2 exhibited an adsorption capacity of 118.1 mg/g for ethyl mercaptan at 500 ppm and a space velocity of 12000 h<sup>−</sup>1, outperforming similar materials reported previously. The high adsorption capacity was attributed to the material’s well-developed microporosity and the abundance of hydroxyl groups (–OH) on its surface, facilitating the chemisorption of ethyl mercaptan. Given the chemically adsorbed nature of sulfur compounds, N<sub>2</sub> thermal regeneration was insufficient to fully recover the adsorbent’s performance. However, oxidative regeneration using O<sub>2</sub>/N<sub>2</sub> (3/97 v/v) at 250 °C successfully removed these compounds and restored desulfurization efficiency, likely due to oxygen-assisted reactions on the adsorbent surface. This study provides valuable insights for effectively treating sulfur-containing odorous gases in the air.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"302 ","pages":"Article 120915"},"PeriodicalIF":4.1,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594180","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
With the acceleration of industrialization, formaldehyde detection is becoming increasingly important. Numerous challenges persist about sensitivity and safety in the field of formaldehyde detection. This paper developed a formaldehyde detection material based on carbon dots, and effectively improved the sensitivity, safety and convenience of detection. Specifically, tannin acid (TA) was utilized as the carbon source and urea as the nitrogen source to prepare tannin/urea carbon dots (TA-CDs) with excellent performance. The fluorescence intensity of the carbon dot solution gradually decreased with increasing formaldehyde concentration. A significant linear relationship (R2 = 0.99462) was observed in the range of 0.00015–0.035 mmol/L, with a practical formaldehyde detection limit of 0.296 μmol/L. This paper utilizes natural poly-phenol compound TA as the raw material, which boasts unique characteristics and low cost. TA-CDs prepared from it are abundant in surface defects and active sites, exhibiting significant advantages in formaldehyde detection and possessing immense application potential.
{"title":"Formaldehyde detection based on tannin carbon dots","authors":"Yaning Li, Chuanxi Chi, Yue Zhao, Guiquan Jiang, Junhua Wu, Jianxi Song","doi":"10.1016/j.ces.2024.120914","DOIUrl":"https://doi.org/10.1016/j.ces.2024.120914","url":null,"abstract":"With the acceleration of industrialization, formaldehyde detection is becoming increasingly important. Numerous challenges persist about sensitivity and safety in the field of formaldehyde detection. This paper developed a formaldehyde detection material based on carbon dots, and effectively improved the sensitivity, safety and convenience of detection. Specifically, tannin acid (TA) was utilized as the carbon source and urea as the nitrogen source to prepare tannin/urea carbon dots (TA-CDs) with excellent performance. The fluorescence intensity of the carbon dot solution gradually decreased with increasing formaldehyde concentration. A significant linear relationship (R<sup>2</sup> = 0.99462) was observed in the range of 0.00015–0.035 mmol/L, with a practical formaldehyde detection limit of 0.296 μmol/L. This paper utilizes natural poly-phenol compound TA as the raw material, which boasts unique characteristics and low cost. TA-CDs prepared from it are abundant in surface defects and active sites, exhibiting significant advantages in formaldehyde detection and possessing immense application potential.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"146 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594181","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 : 2024-11-06DOI: 10.1016/j.ces.2024.120857
Zahra Khani , Joshua Brinkerhoff , Gregory S. Patience
Carbohydrates specified C6 sugars dehydrate to produce platform chemicals like 5-hydroxymethyl furfural and furfural that further oxidize to chemicals 2,5-diformyl furan and 2,5-furan dicarboxylic acid. Here we propose a gas-phase in which a two-fluid nozzle atomizes a 0:1 fructose in water solution into a fluidized bed of Mo–V–/. However, the imperfect interaction between droplet and catalyst increases the agglomeration, which destroys the heat transfer efficiency and hydrodynamic stability. We evaluated the temperature and gas residence time distribution in catalytic bed to improve reaction and process performance by modifying the bed temperature, bed height, and gas velocity. A high mass of catalyst (>) degrades fructose and reduces the selectivity. At temperature distributes homogeneously within bed and with time on process it shifts toward higher values. Velocity in the range of to yields product with the highest selectivity (16%). These results demonstrate the potential of optimizing gas-phase catalytic processes to improve the selective production of platform chemicals from carbohydrates, supporting more sustainable chemical manufacturing.
{"title":"Hydrodynamic and temperature profile analysis in a gas-solid fluidized bed with liquid atomization to convert fructose to value-added chemicals","authors":"Zahra Khani , Joshua Brinkerhoff , Gregory S. Patience","doi":"10.1016/j.ces.2024.120857","DOIUrl":"10.1016/j.ces.2024.120857","url":null,"abstract":"<div><div>Carbohydrates specified C6 sugars dehydrate to produce platform chemicals like 5-hydroxymethyl furfural and furfural that further oxidize to chemicals 2,5-diformyl furan and 2,5-furan dicarboxylic acid. Here we propose a gas-phase in which a two-fluid nozzle atomizes a 0:1 <figure><img></figure> fructose in water solution into a fluidized bed of Mo–V–<figure><img></figure>/<figure><img></figure>. However, the imperfect interaction between droplet and catalyst increases the agglomeration, which destroys the heat transfer efficiency and hydrodynamic stability. We evaluated the temperature and gas residence time distribution in catalytic bed to improve reaction and process performance by modifying the bed temperature, bed height, and gas velocity. A high mass of catalyst (><figure><img></figure>) degrades fructose and reduces the selectivity. At <figure><img></figure> temperature distributes homogeneously within bed and with time on process it shifts toward higher values. Velocity in the range of <figure><img></figure> to <figure><img></figure> yields product with the highest selectivity (16%). These results demonstrate the potential of optimizing gas-phase catalytic processes to improve the selective production of platform chemicals from carbohydrates, supporting more sustainable chemical manufacturing.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"302 ","pages":"Article 120857"},"PeriodicalIF":4.1,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594182","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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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