Engineering surface reaction kinetics plays a vital role in promoting CO2 photoreduction reaction (CO2 PRR) efficiency but remains formidably challenging. Here, we demonstrate that the regulation of the surface oxidation state is an effective strategy for the unification of the adsorption sites and reactive centers, which significantly improves the reaction kinetics and CO2 PRR efficiency. Taking advantage of the concept, we further propose p–p orbital hybridization between P atoms and the adjacent O atoms in BiVO4 at the interface constructed in the O-RP/BiVO4 Z-scheme heterostructure to create the oxidation state of RP. Theoretical calculations and spectral characterizations reveal that the interfacial atomic orbital hybridization lowers the CO2 activation energy barrier through the stabilization of the COOH* intermediate and facilitates the charge separation and transfer. Consequently, the optimized photocatalyst exhibits an excellent performance for sacrificial reagent-free CO2 PRR, with a production rate of 208 and 26.2 μmol g–1 h–1 for CO and CH4, respectively, ca. 21-fold higher than that of pristine RP and topping most of the hybrid photocatalysts with a noble metal as cocatalysts. This work provides critical insight for the design of high-efficiency photocatalysts for CO2 PRR.
{"title":"Improved Surface Reaction Kinetics in Red Phosphorus by Oxidation State for Efficient CO2 Photoreduction","authors":"Tianyue Wang, Jia Liu, Bining Tian, Lulu Yan, Zhanfeng Li, Yue Tian","doi":"10.1021/acs.iecr.4c04377","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c04377","url":null,"abstract":"Engineering surface reaction kinetics plays a vital role in promoting CO<sub>2</sub> photoreduction reaction (CO<sub>2</sub> PRR) efficiency but remains formidably challenging. Here, we demonstrate that the regulation of the surface oxidation state is an effective strategy for the unification of the adsorption sites and reactive centers, which significantly improves the reaction kinetics and CO<sub>2</sub> PRR efficiency. Taking advantage of the concept, we further propose p–p orbital hybridization between P atoms and the adjacent O atoms in BiVO<sub>4</sub> at the interface constructed in the <i>O</i>-RP/BiVO<sub>4</sub> Z-scheme heterostructure to create the oxidation state of RP. Theoretical calculations and spectral characterizations reveal that the interfacial atomic orbital hybridization lowers the CO<sub>2</sub> activation energy barrier through the stabilization of the COOH* intermediate and facilitates the charge separation and transfer. Consequently, the optimized photocatalyst exhibits an excellent performance for sacrificial reagent-free CO<sub>2</sub> PRR, with a production rate of 208 and 26.2 μmol g<sup>–1</sup> h<sup>–1</sup> for CO and CH<sub>4</sub>, respectively, ca. 21-fold higher than that of pristine RP and topping most of the hybrid photocatalysts with a noble metal as cocatalysts. This work provides critical insight for the design of high-efficiency photocatalysts for CO<sub>2</sub> PRR.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"87 4 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570086","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 : 2025-03-05DOI: 10.1021/acs.iecr.4c04518
Seong-rye Kim, Ye-Na Choi, Kwangho Park, Hong-Gyung Lee, Kyung Rok Lee, Hongjin Park, Sungho Yoon, Kwan Young Lee, Kwang-Deog Jung
A Mg-promoted Cu/ZnO/ZrO2/Al2O3 catalyst (CZZAM) was developed for methanol synthesis via CO2 hydrogenation. Incorporating magnesium into the catalyst precursor improved the durability, addressing stability issues in our previously reported Cu/ZnO/ZrO2/Al2O3 (CZZA) catalysts. Comparative evaluations showed that CZZAM outperforms commercial Cu/ZnO/Al2O3 (CZA) and CZZA catalysts, achieving a maximum methanol space–time yield of 0.99 gMeOH·gcat–1·h–1 with a methanol selectivity of 50.6% and a yield of 12.7% under 24,000 mL·gcat–1·h–1 at 260 °C and 5 MPa. In a 60 h test, CZZAM exhibited only a 2.8% decrease in methanol productivity compared to over 9 to 10% declines for CZA and CZZA. Characterizations revealed that Mg addition enhanced Cu nanoparticle dispersion and structural stability. These findings demonstrate that Mg incorporation effectively enhances activity and stability in Cu/ZnO/ZrO2/Al2O3 catalysts for CO2 hydrogenation to methanol.
{"title":"Magnesium-Promoted Catalytic Stability of the Cu/ZnO/ZrO2/Al2O3-MgO Catalyst in CO2 Hydrogenation to Methanol","authors":"Seong-rye Kim, Ye-Na Choi, Kwangho Park, Hong-Gyung Lee, Kyung Rok Lee, Hongjin Park, Sungho Yoon, Kwan Young Lee, Kwang-Deog Jung","doi":"10.1021/acs.iecr.4c04518","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c04518","url":null,"abstract":"A Mg-promoted Cu/ZnO/ZrO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst (CZZAM) was developed for methanol synthesis via CO<sub>2</sub> hydrogenation. Incorporating magnesium into the catalyst precursor improved the durability, addressing stability issues in our previously reported Cu/ZnO/ZrO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> (CZZA) catalysts. Comparative evaluations showed that CZZAM outperforms commercial Cu/ZnO/Al<sub>2</sub>O<sub>3</sub> (CZA) and CZZA catalysts, achieving a maximum methanol space–time yield of 0.99 g<sub>MeOH</sub>·g<sub>cat</sub><sup>–1</sup>·h<sup>–1</sup> with a methanol selectivity of 50.6% and a yield of 12.7% under 24,000 mL·g<sub>cat</sub><sup>–1</sup>·h<sup>–1</sup> at 260 °C and 5 MPa. In a 60 h test, CZZAM exhibited only a 2.8% decrease in methanol productivity compared to over 9 to 10% declines for CZA and CZZA. Characterizations revealed that Mg addition enhanced Cu nanoparticle dispersion and structural stability. These findings demonstrate that Mg incorporation effectively enhances activity and stability in Cu/ZnO/ZrO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> catalysts for CO<sub>2</sub> hydrogenation to methanol.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"30 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546960","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Heavy metal ions in water bodies pose a serious threat to human health and the environment. To overcome this issue, we developed a polymeric quercetin–copper complex (QC) as a novel adsorbent for heavy metal removal. This material was characterized using different techniques. Its structure was also investigated using density functional theory (DFT) calculations, which revealed the formation of a highly stable 2:1 complex between quercetin and Cu2+ ion. The QC polymer exhibited >95% adsorption efficiency for removing heavy metals under acidic and neutral pH conditions. The adsorption capacities were 2.50, 0.77, and 0.54 mmol/g for Cr3+, Hg2+, and Cd2+ ions, respectively, under neutral pH conditions. DFT calculations also indicated high adsorption energies of −34.32, −15.10, and −12.37 eV for Cr3+, Hg2+, and Cd2+, respectively. The QC polymer was easily recovered and reused for removal studies of these metal ions without showing a significant loss in its adsorption capacity.
{"title":"Quercetin–Copper Complexation-Based Porous Polymer for Chromium, Mercury, and Cadmium Metal Ion Adsorption: Experimental and Computational Study","authors":"Raveena, Rahul Kalita, Maku Moronshing, Pratibha Kumari, Kuntal Manna, Rita Kakkar","doi":"10.1021/acs.iecr.4c04523","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c04523","url":null,"abstract":"Heavy metal ions in water bodies pose a serious threat to human health and the environment. To overcome this issue, we developed a polymeric quercetin–copper complex (QC) as a novel adsorbent for heavy metal removal. This material was characterized using different techniques. Its structure was also investigated using density functional theory (DFT) calculations, which revealed the formation of a highly stable 2:1 complex between quercetin and Cu<sup>2+</sup> ion. The QC polymer exhibited >95% adsorption efficiency for removing heavy metals under acidic and neutral pH conditions. The adsorption capacities were 2.50, 0.77, and 0.54 mmol/g for Cr<sup>3+</sup>, Hg<sup>2+</sup>, and Cd<sup>2+</sup> ions, respectively, under neutral pH conditions. DFT calculations also indicated high adsorption energies of −34.32, −15.10, and −12.37 eV for Cr<sup>3+</sup>, Hg<sup>2+</sup>, and Cd<sup>2+</sup>, respectively. The QC polymer was easily recovered and reused for removal studies of these metal ions without showing a significant loss in its adsorption capacity.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"42 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546962","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 : 2025-03-05DOI: 10.1021/acs.iecr.4c04442
Shao-Kang Qian, Xin Ma, Hui Lv, Jun-Yang Yan, Gui-Ping Cao, Peng Gao, Wen-Huan Qiao, Alaaddin M. M. Saeed
Monolithic catalyst has eliminated or weakened the adverse effects on the polymer hydrogenation activity of traditional heterogeneous catalysts. This work delves into the adsorption and activation processes of the benzene ring on the surface of catalyst-active metals. Ni has been introduced into Pd to prepare the PdNi-NCNFs@FN bimetallic catalyst. The active metals Pd and Ni have formed bimetallic nanoparticles, and nickel doping can effectively regulate the adsorption energy of PS benzene ring, promote the desorption of intermediates and catalyst surface renewal, and thus improve the activity of PdNi-NCNFs@FN in hydrogenation (with a TOF of 54.78 gPS/(gPd·h)). The catalyst prepared under optimized conditions showed excellent performance in high-concentration/molecular-weight PS hydrogenation. The catalyst significantly weakens the hindrance of viscosity and conformation effects through the shear thinning of high-speed agitation and the “dragon entangled column” mechanism. PdNi-NCNFs@FN has great potential for industrial applications in expanding the PS hydrogenation industry, increasing PS hydrogenation yield, and preparing high-molecular-weight PCHE.
{"title":"Monolithic PdNi-NCNFs@FN Bimetallic Catalyst for Catalytic Hydrogenation of High-Concentration and High-Molecular-Weight PS","authors":"Shao-Kang Qian, Xin Ma, Hui Lv, Jun-Yang Yan, Gui-Ping Cao, Peng Gao, Wen-Huan Qiao, Alaaddin M. M. Saeed","doi":"10.1021/acs.iecr.4c04442","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c04442","url":null,"abstract":"Monolithic catalyst has eliminated or weakened the adverse effects on the polymer hydrogenation activity of traditional heterogeneous catalysts. This work delves into the adsorption and activation processes of the benzene ring on the surface of catalyst-active metals. Ni has been introduced into Pd to prepare the PdNi-NCNFs@FN bimetallic catalyst. The active metals Pd and Ni have formed bimetallic nanoparticles, and nickel doping can effectively regulate the adsorption energy of PS benzene ring, promote the desorption of intermediates and catalyst surface renewal, and thus improve the activity of PdNi-NCNFs@FN in hydrogenation (with a TOF of 54.78 g<sub>PS</sub>/(g<sub>Pd</sub>·h)). The catalyst prepared under optimized conditions showed excellent performance in high-concentration/molecular-weight PS hydrogenation. The catalyst significantly weakens the hindrance of viscosity and conformation effects through the shear thinning of high-speed agitation and the “dragon entangled column” mechanism. PdNi-NCNFs@FN has great potential for industrial applications in expanding the PS hydrogenation industry, increasing PS hydrogenation yield, and preparing high-molecular-weight PCHE.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"3 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560976","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 : 2025-03-05DOI: 10.1021/acs.iecr.4c04776
Wei Li, Bangfu Huang, Xinchao Fan, Keying Zhu, Fu Yuan, Yihang Shi, Zhe Shi, Linjing Yang, Kui Zheng
In order to investigate the nucleation thermodynamics and nucleation kinetics of (NH4)2SO4 during cooling crystallization under the synergistic effect of different ratios of NH4F and NH4Cl, the solubility and width of the metastable zone width of (NH4)2SO4 in the mixed solution were determined by gravimetric and laser methods by incorporation of (NH4)2SO4 in a mixture of different ratios of NH4F and NH4Cl in this study. It is demonstrated that the dissolution of (NH4)2SO4 is a heat-absorbing process, that the inhibition of (NH4)2SO4 nucleation by NH4F is much greater, and that the intermediate stabilization zone of (NH4)2SO4 is enlarged with an increase in the cooling rate. Based on the self-consistent Nývlt-like equation and the classical three-dimensional nucleation theory, the nucleation kinetics of (NH4)2SO4 under the synergistic interaction of NH4F and NH4Cl was investigated, and the critical nucleation parameters of (NH4)2SO4 under the synergistic interaction of NH4F and NH4Cl were obtained.
{"title":"Nucleation Thermodynamics and Nucleation Kinetics of Ammonium Sulfate under the Synergistic Action of Ammonium Chloride and Ammonium Fluoride","authors":"Wei Li, Bangfu Huang, Xinchao Fan, Keying Zhu, Fu Yuan, Yihang Shi, Zhe Shi, Linjing Yang, Kui Zheng","doi":"10.1021/acs.iecr.4c04776","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c04776","url":null,"abstract":"In order to investigate the nucleation thermodynamics and nucleation kinetics of (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> during cooling crystallization under the synergistic effect of different ratios of NH<sub>4</sub>F and NH<sub>4</sub>Cl, the solubility and width of the metastable zone width of (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> in the mixed solution were determined by gravimetric and laser methods by incorporation of (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> in a mixture of different ratios of NH<sub>4</sub>F and NH<sub>4</sub>Cl in this study. It is demonstrated that the dissolution of (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> is a heat-absorbing process, that the inhibition of (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> nucleation by NH<sub>4</sub>F is much greater, and that the intermediate stabilization zone of (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> is enlarged with an increase in the cooling rate. Based on the self-consistent Nývlt-like equation and the classical three-dimensional nucleation theory, the nucleation kinetics of (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> under the synergistic interaction of NH<sub>4</sub>F and NH<sub>4</sub>Cl was investigated, and the critical nucleation parameters of (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> under the synergistic interaction of NH<sub>4</sub>F and NH<sub>4</sub>Cl were obtained.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"45 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546961","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 : 2025-03-05DOI: 10.1021/acs.iecr.5c00110
Mei Lu, Shengdi Wang, Min Su, Zhenghui Weng, Jiawen Zheng, Navneet Kumar Gupta, Kejian Cai, Zhoupeng Shou, Quanli Ke
Plastic waste, particularly the dominant polyolefins, presents a growing environmental issue due to its chemical stability and low recycling rates. Although various methods are proposed to address plastic waste, the strong carbon–carbon bonds within polyolefins, as well as the degradation of mechanical strength and additional value by conventional recycling methods, pose great challenges to their downstream usage. With this regard, this paper emphasizes the chemical recycling of polyolefins into renewable resources, including carbon materials, liquid fuels, and various hydrocarbon chemicals, by thermal catalytic methods. An in-depth discussion on the feasibility and limitations of promising chemical recycling techniques is provided, such as the association between the reactor design, process optimization, catalyst preparation, and the product distribution. Specifically, the structure–function relationship over different catalysts was highlighted, including the molecular sieve, precious metal, transition metal, and ion liquid. In addition, the future challenge regarding the simultaneous treatment of mixed plastics is also summarized, along with the copyrolysis of waste plastic and biomass. As such, this paper underscores sustainable and scalable solutions for polyolefin upcycling, which may shed light upon the industrial application of plastic resources.
{"title":"Insights into Chemical Recycling and Upgrading Strategies for Polyolefin-Based Plastics","authors":"Mei Lu, Shengdi Wang, Min Su, Zhenghui Weng, Jiawen Zheng, Navneet Kumar Gupta, Kejian Cai, Zhoupeng Shou, Quanli Ke","doi":"10.1021/acs.iecr.5c00110","DOIUrl":"https://doi.org/10.1021/acs.iecr.5c00110","url":null,"abstract":"Plastic waste, particularly the dominant polyolefins, presents a growing environmental issue due to its chemical stability and low recycling rates. Although various methods are proposed to address plastic waste, the strong carbon–carbon bonds within polyolefins, as well as the degradation of mechanical strength and additional value by conventional recycling methods, pose great challenges to their downstream usage. With this regard, this paper emphasizes the chemical recycling of polyolefins into renewable resources, including carbon materials, liquid fuels, and various hydrocarbon chemicals, by thermal catalytic methods. An in-depth discussion on the feasibility and limitations of promising chemical recycling techniques is provided, such as the association between the reactor design, process optimization, catalyst preparation, and the product distribution. Specifically, the structure–function relationship over different catalysts was highlighted, including the molecular sieve, precious metal, transition metal, and ion liquid. In addition, the future challenge regarding the simultaneous treatment of mixed plastics is also summarized, along with the copyrolysis of waste plastic and biomass. As such, this paper underscores sustainable and scalable solutions for polyolefin upcycling, which may shed light upon the industrial application of plastic resources.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"131 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546963","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 : 2025-03-04DOI: 10.1021/acs.iecr.4c04612
Qifan Li, Yi Zheng, Fangxiao Li
Enhancing the heat transfer performance of porous structures through effective control of wettability and surface morphology has emerged as a critical factor in ensuring efficient equipment operation under high power conditions. This paper investigates the dynamic behavior of bubble growth on porous surfaces by establishing a transient fluid continuum surface force (VOF-CSF) model, emphasizing how wettability and surface microstructure influence bubble dynamics with specific wettability and microcavity configurations. The results indicate that the adhesion effect associated with hydrophobic surfaces leads to bubbles primarily expanding in the horizontal direction, thereby facilitating their merging with adjacent bubbles. As for smooth hydrophilic porous surfaces, there exists a clear microlayer liquid film between the bubbles and particles and replenishes the liquid supply. While, the microcavity structures generate numerous vortices at the bottom of the liquid film that significantly disturb the vapor–liquid interface and significantly enhance bubble departure; additionally, the liquid film within these microcavities provides an effective rehydration pathway. Furthermore, the microclusters induced by the fluid continuously interact with the bubble boundary, significantly enhancing the growth behavior of the bubbles. This interaction results in an increase in the bubble growth rate by 30–40% and improves heat transfer performance within porous structures by 23%.
{"title":"Study on the Mechanism of Bubble Transport on Porous Structure Controlled by Surface Wettability and Microcavity","authors":"Qifan Li, Yi Zheng, Fangxiao Li","doi":"10.1021/acs.iecr.4c04612","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c04612","url":null,"abstract":"Enhancing the heat transfer performance of porous structures through effective control of wettability and surface morphology has emerged as a critical factor in ensuring efficient equipment operation under high power conditions. This paper investigates the dynamic behavior of bubble growth on porous surfaces by establishing a transient fluid continuum surface force (VOF-CSF) model, emphasizing how wettability and surface microstructure influence bubble dynamics with specific wettability and microcavity configurations. The results indicate that the adhesion effect associated with hydrophobic surfaces leads to bubbles primarily expanding in the horizontal direction, thereby facilitating their merging with adjacent bubbles. As for smooth hydrophilic porous surfaces, there exists a clear microlayer liquid film between the bubbles and particles and replenishes the liquid supply. While, the microcavity structures generate numerous vortices at the bottom of the liquid film that significantly disturb the vapor–liquid interface and significantly enhance bubble departure; additionally, the liquid film within these microcavities provides an effective rehydration pathway. Furthermore, the microclusters induced by the fluid continuously interact with the bubble boundary, significantly enhancing the growth behavior of the bubbles. This interaction results in an increase in the bubble growth rate by 30–40% and improves heat transfer performance within porous structures by 23%.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"99 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539132","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Utilization of polyethylene (PE) has caused serious white pollution. Degradation of PE-based wastes has been a great concern. The traditional pyrolysis strategy for degrading PE-based wastes has problems, including operation temperature being higher than 200 °C and products being complex mixtures. Herein, PE is first degraded into CO2 and H2 at room temperature lower than 33 °C via a room-temperature discharge-driven degradation (RT-DD) process, with a degradation rate as high as 7.6 kg h–1 m–2. Then, the CO2 and H2 formed from the RT-DD process are converted into CO on a molybdenum carbide-based catalyst at 450 °C, with a CO selectivity of 100%. The RT-DD process effectively breaks and thoroughly oxidizes PE chains through the generation of high-energy electrons, oxygen radicals, and other active species. Moreover, through parallel connection, RT-DD reactors can be easily assembled into a larger system with the area of the working zone reaching 1 m2. This offers a great potential for commercialization.
{"title":"Boosting Degradation of Polyethylene at Room Temperature","authors":"Yiyi Zhao, Peng Liu, Xin-Yu Meng, Yu-Long Men, Hongmin Ma, Jiafu Zou, Tingwei Wang, Yun-Xiang Pan","doi":"10.1021/acs.iecr.4c04725","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c04725","url":null,"abstract":"Utilization of polyethylene (PE) has caused serious white pollution. Degradation of PE-based wastes has been a great concern. The traditional pyrolysis strategy for degrading PE-based wastes has problems, including operation temperature being higher than 200 °C and products being complex mixtures. Herein, PE is first degraded into CO<sub>2</sub> and H<sub>2</sub> at room temperature lower than 33 °C via a room-temperature discharge-driven degradation (RT-DD) process, with a degradation rate as high as 7.6 kg h<sup>–1</sup> m<sup>–2</sup>. Then, the CO<sub>2</sub> and H<sub>2</sub> formed from the RT-DD process are converted into CO on a molybdenum carbide-based catalyst at 450 °C, with a CO selectivity of 100%. The RT-DD process effectively breaks and thoroughly oxidizes PE chains through the generation of high-energy electrons, oxygen radicals, and other active species. Moreover, through parallel connection, RT-DD reactors can be easily assembled into a larger system with the area of the working zone reaching 1 m<sup>2</sup>. This offers a great potential for commercialization.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"130 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539131","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 : 2025-03-04DOI: 10.1021/acs.iecr.4c04543
F.-Y. Jou, A. E. Mather, K. A. G. Schmidt
The solubility of dimethyl sulfide in liquid solvents is of considerable interest to the chemical, natural gas, petroleum, food, and pulp and paper industries. There are limited data in the open literature for the solubility of dimethyl sulfide in water at elevated temperatures and pressures. The gaps in the literature data were addressed with new experimental solubility measurements at temperatures in the range (298.15–413.15) K over a wide range of dimethyl sulfide partial pressures. The cubic-plus-association equation of state was used to correlate the new and existing data with a temperature-dependent binary interaction parameter. Henry’s law constants were correlated with temperature over the full temperature range with a Clarke–Glew smoothing equation.
{"title":"Solubility of Dimethyl Sulfide in Water","authors":"F.-Y. Jou, A. E. Mather, K. A. G. Schmidt","doi":"10.1021/acs.iecr.4c04543","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c04543","url":null,"abstract":"The solubility of dimethyl sulfide in liquid solvents is of considerable interest to the chemical, natural gas, petroleum, food, and pulp and paper industries. There are limited data in the open literature for the solubility of dimethyl sulfide in water at elevated temperatures and pressures. The gaps in the literature data were addressed with new experimental solubility measurements at temperatures in the range (298.15–413.15) K over a wide range of dimethyl sulfide partial pressures. The cubic-plus-association equation of state was used to correlate the new and existing data with a temperature-dependent binary interaction parameter. Henry’s law constants were correlated with temperature over the full temperature range with a Clarke–Glew smoothing equation.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"36 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546965","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Styrene–butadiene rubber (SBR), a widely employed synthetic elastomer, has found diverse applications, including transportation, sealing, and conveyor belts. Nevertheless, the conventional covalent cross-linking network inherently restricts its recyclability and reprocessability, leading to substantial resource depletion and considerable environmental degradation. Herein, we present an efficient strategy for the fabrication of high-performance and recyclable SBR materials based on ionic cluster interactions. The commercial SBR is brominated to establish dynamic ionic cluster cross-linking networks with 4-(alkylamino)-pyridine (DMAP) under simple hot pressing condition. Owing to the electron-donating characteristics and resonance-induced isomerization of DMAP, the SBR obtained in this study attains a markedly elevated tensile strength of 12.0 MPa and a toughness of 48.9 MJ/m3, both of which outperform those of conventional sulfur-vulcanized SBR. Furthermore, the developed SBR materials exhibit outstanding reprocessability due to their effective reversibility of dynamic bromine-DMAP ionic cluster cross-linking, endowing the rubber materials with good recyclability. This study proposes an effective methodology for the fabrication of high-performance, recyclable elastomeric materials, paving a promising path for the sustainable advancement of the rubber industry.
{"title":"Mechanically Robust and Recyclable Styrene–Butadiene Rubber Realized by Ion Cluster Dynamic Cross-Link","authors":"Changwei Wu, Zhengtian Xie, Jie Wen, Xinyuan Bi, Pengfei Lv, Yuanyuan Dou, Chao Wang, Jinrong Wu","doi":"10.1021/acs.iecr.5c00310","DOIUrl":"https://doi.org/10.1021/acs.iecr.5c00310","url":null,"abstract":"Styrene–butadiene rubber (SBR), a widely employed synthetic elastomer, has found diverse applications, including transportation, sealing, and conveyor belts. Nevertheless, the conventional covalent cross-linking network inherently restricts its recyclability and reprocessability, leading to substantial resource depletion and considerable environmental degradation. Herein, we present an efficient strategy for the fabrication of high-performance and recyclable SBR materials based on ionic cluster interactions. The commercial SBR is brominated to establish dynamic ionic cluster cross-linking networks with 4-(alkylamino)-pyridine (DMAP) under simple hot pressing condition. Owing to the electron-donating characteristics and resonance-induced isomerization of DMAP, the SBR obtained in this study attains a markedly elevated tensile strength of 12.0 MPa and a toughness of 48.9 MJ/m<sup>3</sup>, both of which outperform those of conventional sulfur-vulcanized SBR. Furthermore, the developed SBR materials exhibit outstanding reprocessability due to their effective reversibility of dynamic bromine-DMAP ionic cluster cross-linking, endowing the rubber materials with good recyclability. This study proposes an effective methodology for the fabrication of high-performance, recyclable elastomeric materials, paving a promising path for the sustainable advancement of the rubber industry.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"84 1","pages":""},"PeriodicalIF":4.2,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546970","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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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