Pub Date : 2025-01-27DOI: 10.1016/j.cej.2025.160010
Jun Xiao, Hong Gao, Yang Xiao, Shijian Wang, Cheng Gong, Zefu Huang, Bing Sun, Chung-Li Dong, Xin Guo, Hao Liu, Guoxiu Wang
A dual-site substitution strategy was applied to enhance the electrochemical performance of sodium-ion batteries, leading to the development of the Na0.80Mg0.03Li0.18Mn0.67Cu0.15O2 cathode material. By introducing Mg and Cu ions at multiple sites, the local chemical environment was optimized, resulting in improved ion diffusion kinetics and charge transfer dynamics, which accelerate the overall electrochemical reactions. Mg ions substituted at Na sites act as “pillars” effectively mitigating detrimental O2−–O2− electrostatic repulsion and enabling stable anion redox activity. This novel cathode demonstrates a high specific capacity of 162 mAh/g, excellent rate capability with 114 mAh/g at 1000 mA g−1 (8C), and superior cycling stability with 80.3 % capacity retention after 300 cycles. Furthermore, the dual-site substitution minimizes volume variation to just 1.3 % during electrochemical processes and significantly enhances moisture resistance, offering promising potential for practical sodium-ion battery applications.
{"title":"A hydro-stable and phase-transition-free P2-type cathode with superior cycling stability for high-voltage sodium-ion batteries","authors":"Jun Xiao, Hong Gao, Yang Xiao, Shijian Wang, Cheng Gong, Zefu Huang, Bing Sun, Chung-Li Dong, Xin Guo, Hao Liu, Guoxiu Wang","doi":"10.1016/j.cej.2025.160010","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160010","url":null,"abstract":"A dual-site substitution strategy was applied to enhance the electrochemical performance of sodium-ion batteries, leading to the development of the Na<sub>0.80</sub>Mg<sub>0.03</sub>Li<sub>0.18</sub>Mn<sub>0.67</sub>Cu<sub>0.15</sub>O<sub>2</sub> cathode material. By introducing Mg and Cu ions at multiple sites, the local chemical environment was optimized, resulting in improved ion diffusion kinetics and charge transfer dynamics, which accelerate the overall electrochemical reactions. Mg ions substituted at Na sites act as “pillars” effectively mitigating detrimental O<sup>2−</sup>–O<sup>2−</sup> electrostatic repulsion and enabling stable anion redox activity. This novel cathode demonstrates a high specific capacity of 162 mAh/g, excellent rate capability with 114 mAh/g at 1000 mA g<sup>−1</sup> (8C), and superior cycling stability with 80.3 % capacity retention after 300 cycles. Furthermore, the dual-site substitution minimizes volume variation to just 1.3 % during electrochemical processes and significantly enhances moisture resistance, offering promising potential for practical sodium-ion battery applications.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"59 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050584","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Solar interfacial photothermal-catalytic water evaporation is an emerging method for obtaining clean water from polluted water. However, many studies overlook the crucial aspect of clean water recovery. This study develops an interfacial photothermal-catalytic water evaporator (Carbon felt/TiO2-Expandable polyethylene, CF/TiO2-EPE) inspired by the “ship-in-a-bottle”. The strategy confines TiO2 to the pore structure of CF to maintain its nanoscale size and form a macroscale structure, providing more reaction sites for photocatalysis and increasing the number of incident light reflections. Additionally, the reduction of CF pore size enhances the capillary effect, resulting in stable water transport. These characteristics endow CF/TiO2-EPE with excellent photothermal synergistic purification performance. Specifically, CF/TiO2-EPE removes 92.5 % of the antibiotic ciprofloxacin from wastewater. Meanwhile, a novel evaporation device is designed to enhance vapor escape and collection through micro-airflow, reducing the loss of light and heat energy, resulting in a clean water yield of up to 1.81 kg m-2h−1. Compared to traditional water evaporation devices, its clean water recovery rate increased by 10.5 times and 13.7 times, respectively. Furthermore, this photothermal-catalytic water evaporation system can produce 46.43 kg m−2 of clean water under 24-hour continuous operation with low energy consumption, sufficient to meet the daily water needs of 11 adults. The rational design of photothermal-catalytic structures and the development of new water evaporation devices are of great importance for obtaining clean water from polluted water efficiently and sustainably.
{"title":"Rational design of “ship-in-a-bottle” evaporator with integrated solar evaporation and photocatalytic degradation for sustainable water treatment","authors":"Hongyang Guo, Ting Zhang, Xiaoman Zhang, Cuijiao Mao, Xiaodan Liu, Shuqi Wan, Qilu Li, Jianhui Sun, Shuying Dong, Chongfei Yu, Yongfa Zhu","doi":"10.1016/j.cej.2025.159995","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159995","url":null,"abstract":"Solar interfacial photothermal-catalytic water evaporation is an emerging method for obtaining clean water from polluted water. However, many studies overlook the crucial aspect of clean water recovery. This study develops an interfacial photothermal-catalytic water evaporator (Carbon felt/TiO<sub>2</sub>-Expandable polyethylene, CF/TiO<sub>2</sub>-EPE) inspired by the “ship-in-a-bottle”. The strategy confines TiO<sub>2</sub> to the pore structure of CF to maintain its nanoscale size and form a macroscale structure, providing more reaction sites for photocatalysis and increasing the number of incident light reflections. Additionally, the reduction of CF pore size enhances the capillary effect, resulting in stable water transport. These characteristics endow CF/TiO<sub>2</sub>-EPE with excellent photothermal synergistic purification performance. Specifically, CF/TiO<sub>2</sub>-EPE removes 92.5 % of the antibiotic ciprofloxacin from wastewater. Meanwhile, a novel evaporation device is designed to enhance vapor escape and collection through micro-airflow, reducing the loss of light and heat energy, resulting in a clean water yield of up to 1.81 kg m<sup>-2</sup>h<sup>−1</sup>. Compared to traditional water evaporation devices, its clean water recovery rate increased by 10.5 times and 13.7 times, respectively. Furthermore, this photothermal-catalytic water evaporation system can produce 46.43 kg m<sup>−2</sup> of clean water under 24-hour continuous operation with low energy consumption, sufficient to meet the daily water needs of 11 adults. The rational design of photothermal-catalytic structures and the development of new water evaporation devices are of great importance for obtaining clean water from polluted water efficiently and sustainably.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"148 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050601","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-27DOI: 10.1016/j.cej.2025.160004
Zhi Chen, Yingnan Hua, Bing Chen, Jiwen Feng, Gang Liu, Bin Jiang
MOFs (metal–organic frameworks) have large specific surface area, abundant active sites, and tunable pore structures, making them highly attractive anode materials for lithium-ion batteries. However, their inadequate electrical conductivity and rate performance greatly hinder the further applications of MOFs in field of energy storage. In this study, we present a robust Mn-MOF/HA (humic acid) composite anode material with multilayer nano-sheet structures, synthesized via in-situ compositing HA with Mn-MOF in general hydrothermal reaction. The Mn-MOF derived from hydrothermal reaction shows poor electrochemical stability and low electrical conductivity. The incorporation of HA notably elevates electrochemical stability of materials, boosts both electrical and lithium-ion conductivity, and also modulates the microstructure to form ultrathin multilayer nanosheets by rationally adjusting the feed ratio of HA. The resulting HA20-Mn-MOF (with a HA feed ratio of 20 %) demonstrates significant improvements in cycling stability and rate performance, with a reversible specific capacity of 1318.7mAh/g at 0.1 A/g after 100 cycles and a substantial capacity of 657.0mAh/g even after 1000 cycles at 1 A/g. An extraordinary V-shaped capacity reversal is observed for HA20-Mn-MOF during cycling. Ex-situ EPR (Electron Paramagnetic Resonance) investigation reveals this capacity growth is associated with the reoxidation of active manganese during cycling, in which a notable correlation between the specific capacity and the Mn2+ signal intensity in EPR spectra is found. These results suggest in-situ compositing HA with MOFs can be a cost-effective strategy in regulating MOFs morphology and in achieving an optimized electrochemical performance for MOFs-based electrode materials in energy storage field.
{"title":"In-situ compositing HA significantly enhancing electrochemical performance of Mn-MOF anode materials","authors":"Zhi Chen, Yingnan Hua, Bing Chen, Jiwen Feng, Gang Liu, Bin Jiang","doi":"10.1016/j.cej.2025.160004","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160004","url":null,"abstract":"MOFs (metal–organic frameworks) have large specific surface area, abundant active sites, and tunable pore structures, making them highly attractive anode materials for lithium-ion batteries. However, their inadequate electrical conductivity and rate performance greatly hinder the further applications of MOFs in field of energy storage. In this study, we present a robust Mn-MOF/HA (humic acid) composite anode material with multilayer nano-sheet structures, synthesized via in-situ compositing HA with Mn-MOF in general hydrothermal reaction. The Mn-MOF derived from hydrothermal reaction shows poor electrochemical stability and low electrical conductivity. The incorporation of HA notably elevates electrochemical stability of materials, boosts both electrical and lithium-ion conductivity, and also modulates the microstructure to form ultrathin multilayer nanosheets by rationally adjusting the feed ratio of HA. The resulting HA<sub>20</sub>-Mn-MOF (with a HA feed ratio of 20 %) demonstrates significant improvements in cycling stability and rate performance, with a reversible specific capacity of 1318.7mAh/g at 0.1 A/g after 100 cycles and a substantial capacity of 657.0mAh/g even after 1000 cycles at 1 A/g. An extraordinary V-shaped capacity reversal is observed for HA<sub>20</sub>-Mn-MOF during cycling. Ex-situ EPR (Electron Paramagnetic Resonance) investigation reveals this capacity growth is associated with the reoxidation of active manganese during cycling, in which a notable correlation between the specific capacity and the Mn<sup>2+</sup> signal intensity in EPR spectra is found. These results suggest in-situ compositing HA with MOFs can be a cost-effective strategy in regulating MOFs morphology and in achieving an optimized electrochemical performance for MOFs-based electrode materials in energy storage field.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"35 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050755","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Rotator cuff injury is a common shoulder disease, which can lead to severe shoulder pain and functional limitation. The natural healing process of tendon-bone after rotator cuff injury is slow and often ineffective, and the long-term stress concentration at the injured tendon-bone interface will lead to the re-tear of the healed tissue. Therefore, the development of biomaterials that can provide mechanical support and induce synchronous multitissue regeneration at the tendon-bone interface is a priority. In this study, PCL and COL Ⅰ were blended by electrospinning technology to prepare nanofiber patches with bionic mechanical properties, including sufficient tensile strength and significant elasticity, and multifunctional composite patches were prepared by loading CaSiO3 and CTGF onto the patches through a double-ended loading strategy. The multifunctional patch has good biocompatibility, and has shown significant advantages in promoting multitissue regeneration. The application of multifunctional patch in rat rotator cuff injury model can effectively promote the regeneration of tendon, cartilage and bone at the tendon-bone interface, and simultaneously complete the healing of tendon to bone, which has a significant effect on promoting the repair of rotator cuff injury. Our study demonstrates the great potential of patch materials for gradient tissue repair and provides a feasible strategy for multi-tissue induced electrospinning scaffolds for the regeneration of the soft-hard tissue interface.
{"title":"Biomimetic patch with gradient-induced regeneration for tendon-bone interface to repair rotator cuff injury","authors":"Jinshan Jiang, Jinpeng Wan, Xinyi Yu, Xin Yi, Weizhen Hu, Miao Gu, Jianke Huo, Weichao Dai, Haicui Yao, Dongdong Wan, Zhenyu Zhou, Shufang Wang","doi":"10.1016/j.cej.2025.159985","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159985","url":null,"abstract":"Rotator cuff injury is a common shoulder disease, which can lead to severe shoulder pain and functional limitation. The natural healing process of tendon-bone after rotator cuff injury is slow and often ineffective, and the long-term stress concentration at the injured tendon-bone interface will lead to the re-tear of the healed tissue. Therefore, the development of biomaterials that can provide mechanical support and induce synchronous multitissue regeneration at the tendon-bone interface is a priority. In this study, PCL and COL Ⅰ were blended by electrospinning technology to prepare nanofiber patches with bionic mechanical properties, including sufficient tensile strength and significant elasticity, and multifunctional composite patches were prepared by loading CaSiO<sub>3</sub> and CTGF onto the patches through a double-ended loading strategy. The multifunctional patch has good biocompatibility, and has shown significant advantages in promoting multitissue regeneration. The application of multifunctional patch in rat rotator cuff injury model can effectively promote the regeneration of tendon, cartilage and bone at the tendon-bone interface, and simultaneously complete the healing of tendon to bone, which has a significant effect on promoting the repair of rotator cuff injury. Our study demonstrates the great potential of patch materials for gradient tissue repair and provides a feasible strategy for multi-tissue induced electrospinning scaffolds for the regeneration of the soft-hard tissue interface.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"15 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050786","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-27DOI: 10.1016/j.cej.2025.159969
Ao Huang, Nan Zhang, Qian-Bin Wang, Bo-Han Zhao, Rui-Bao Zhang, Ming Cheng, Chen Shi, Xiao-Di Hao
With industrialization advances, the volume of wastewater produced has increased considerably. In recent years, biochar-loaded layered double hydroxides (BC–LDHs) have emerged as a low-cost, sustainable composite material with promising applications in wastewater treatment. Improving the adsorption performance of materials is a central focus in the field of wastewater treatment. Currently, most studies emphasize the adsorption applications of BC–LDHs. However, this study not only discusses existing mainstream methods for enhancing adsorption performance but also shifts the focus from BC modification to LDH synthesis. Building on this, new potential modification methods are proposed to achieve improved adsorption performance. One such method involves obtaining new anion-intercalated BC–LDHs through ion exchange. Another approach is to synthesize BC–LDHs via electrodeposition, which involves using an LDH as the working electrode and then loading BC onto it or using BC as one of the electrodes with a mixed metal salt solution as the electrolyte. Different synthesis methods often result in distinct material properties. The electrodeposition method is used to synthesize BC–LDHs with the aim of achieving material modification. In addition, the factors influencing BC–LDHs are analyzed. Through meta-analysis, the study identifies notable factors affecting the adsorption properties of pollutants, including different synthesis methods, the specific surface area of BC–LDHs, adsorbent dosage, and initial pH. This analysis offers a more intuitive foundation for guiding subsequent research by focusing on these critical factors. Finally, the main adsorption mechanism of BC–LDHs is summarized, and future research directions for BC–LDHs are proposed.
{"title":"Enhanced wastewater treatment using biochar-supported layered-double-hydroxide composites","authors":"Ao Huang, Nan Zhang, Qian-Bin Wang, Bo-Han Zhao, Rui-Bao Zhang, Ming Cheng, Chen Shi, Xiao-Di Hao","doi":"10.1016/j.cej.2025.159969","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159969","url":null,"abstract":"With industrialization advances, the volume of wastewater produced has increased considerably. In recent years, biochar-loaded layered double hydroxides (BC–LDHs) have emerged as a low-cost, sustainable composite material with promising applications in wastewater treatment. Improving the adsorption performance of materials is a central focus in the field of wastewater treatment. Currently, most studies emphasize the adsorption applications of BC–LDHs. However, this study not only discusses existing mainstream methods for enhancing adsorption performance but also shifts the focus from BC modification to LDH synthesis. Building on this, new potential modification methods are proposed to achieve improved adsorption performance. One such method involves obtaining new anion-intercalated BC–LDHs through ion exchange. Another approach is to synthesize BC–LDHs via electrodeposition, which involves using an LDH as the working electrode and then loading BC onto it or using BC as one of the electrodes with a mixed metal salt solution as the electrolyte. Different synthesis methods often result in distinct material properties. The electrodeposition method is used to synthesize BC–LDHs with the aim of achieving material modification. In addition, the factors influencing BC–LDHs are analyzed. Through <em>meta</em>-analysis, the study identifies notable factors affecting the adsorption properties of pollutants, including different synthesis methods, the specific surface area of BC–LDHs, adsorbent dosage, and initial pH. This analysis offers a more intuitive foundation for guiding subsequent research by focusing on these critical factors. Finally, the main adsorption mechanism of BC–LDHs is summarized, and future research directions for BC–LDHs are proposed.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"59 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050780","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-27DOI: 10.1016/j.cej.2025.160028
Wenwen Chen, Haoyong Li, Chuanqi Liu, Yiqun Li, Dezhi Sun, Bin Qiu, Pengsong Li, Haiyu Xu, Hongbin Wu, Yan Dang
The low pH and intricate pollutants in Chinese liquor brewing wastewater (CLBW) pose significant challenges for effective anaerobic digestion (AD) treatment. Granular activated carbon (GAC) can facilitate direct interspecies electron transfer (DIET) and enhance the system’s tolerance to high OLR and low pH. This study investigates a novel approach combining GAC addition and slight influent pH adjustment, which can enhance AD performance of CLBW with reduced alkali need. The synergistic effects and underlying mechanisms remain unclear. The results revealed that the reactor (R20-1), amended with 20 g/L GAC and the influent pH adjusted by adding 1 g NaOH/Linfluent, while the non-GAC reactor failed rapidly at an initial OLR of 3.4 kg COD/(m3∙d). Microbial community analysis revealed that Prevotella was enriched at 12.7 kg COD/(m3∙d)), whereas Parabacteroides dominated at high OLRs > 15.9 kg COD/(m3∙d). Key archaea such as Methanobacterium and Methanosaeta were predominant, with Methanocorpusculum and Methanobrevibacter enriched at high OLRs. Electroactive bacteria, particularly Syntrophomonas, were enriched in R20-1 but decreased at high OLRs. Moreover, genes involved in both DIET and acetate decarboxylation pathways assigned to Methanosaeta showed increased expression with GAC addition. This research provides valuable insights into microbial evolution, functional gene changes and the correlation relationships among environmental factors and microorganisms with increasing OLR, offering a more cost-saving and efficient strategy for treating high-strength organic and acidic wastewater compared to traditional AD methods.
{"title":"Optimizing anaerobic digestion of Chinese liquor brewing wastewater: A cost-effective and high-performance approach","authors":"Wenwen Chen, Haoyong Li, Chuanqi Liu, Yiqun Li, Dezhi Sun, Bin Qiu, Pengsong Li, Haiyu Xu, Hongbin Wu, Yan Dang","doi":"10.1016/j.cej.2025.160028","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160028","url":null,"abstract":"The low pH and intricate pollutants in Chinese liquor brewing wastewater (CLBW) pose significant challenges for effective anaerobic digestion (AD) treatment. Granular activated carbon (GAC) can facilitate direct interspecies electron transfer (DIET) and enhance the system’s tolerance to high OLR and low pH. This study investigates a novel approach combining GAC addition and slight influent pH adjustment, which can enhance AD performance of CLBW with reduced alkali need. The synergistic effects and underlying mechanisms remain unclear. The results revealed that the reactor (R20-1), amended with 20 g/L GAC and the influent pH adjusted by adding 1 g NaOH/L<sub>influent</sub>, while the non-GAC reactor failed rapidly at an initial OLR of 3.4 kg COD/(m<sup>3</sup>∙d). Microbial community analysis revealed that <em>Prevotella</em> was enriched at 12.7 kg COD/(m<sup>3</sup>∙d)), whereas <em>Parabacteroides</em> dominated at high OLRs > 15.9 kg COD/(m<sup>3</sup>∙d). Key archaea such as <em>Methanobacterium</em> and <em>Methanosaeta</em> were predominant, with <em>Methanocorpusculum</em> and <em>Methanobrevibacter</em> enriched at high OLRs. Electroactive bacteria, particularly <em>Syntrophomonas</em>, were enriched in R20-1 but decreased at high OLRs. Moreover, genes involved in both DIET and acetate decarboxylation pathways assigned to <em>Methanosaeta</em> showed increased expression with GAC addition. This research provides valuable insights into microbial evolution, functional gene changes and the correlation relationships among environmental factors and microorganisms with increasing OLR, offering a more cost-saving and efficient strategy for treating high-strength organic and acidic wastewater compared to traditional AD methods.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"119 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050789","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Biocatalytic activity of artificial nanozymes is strongly correlated with the detection sensitivity of lateral flow immunoassays (LFIA). Modulating the electronic structure is a promising and effective strategy to improve the catalytic activity of nanozymes, but remains a challenge. In this study, we develop a single-atom nanozyme LFIA platform with high active and electron-rich Pt single atoms onto AuPd support (Pt1/PA). The Pt1/PA nanozymes exhibit superior peroxidase (POD)-like activity with the catalytic efficiency (Kcat/Km) of 9.29 × 106 mM−1·min−1, which is 315-fold higher than natural horseradish peroxidase (HRP). Density Functional Theory calculations reveal that the remarkable activity is attributed to the formation of electron-rich site of Pt single atoms through electron transfer from support to Pt 5d orbitals, as well as d-band center modulation. Moreover, more electron transfer numbers are available for Pt single atoms at the surface in the lattice than outside the lattice. Benefiting from excellent biocatalytic activity, the limits of detection (LOD) of Pt1/PA-LFIA for carcinoembryonic antigen (CEA) and prostate-specific antigen (PSA) are 1.21pg mL−1 and 0.6pg mL−1, which are 20.4 and 13.3-fold lower than commercial enzyme-linked immunosorbent assay kits (CEA: ab264604, 24.68pg mL−1; PSA: ab264615, 8pg mL−1), respectively. More importantly, Pt1/PA-LFIA achieves the accurate detection of prostate cancer and lung cancer clinical patients. This work presents a paradigm for ultrasensitive biomarker diagnostics based on single-atom nanozyme immunoassays.
{"title":"Single-atom nanozyme immunoassay with electron-rich property for clinical patient cancer detection","authors":"Qingshan Liu, Guo Li, Yang Cao, Yaoyao Ren, Qiong Qin, Lei Li, Hao Zhang, Qi Xin, Xiaoqun Gong, Lingyu Zhao, Shu Zhang, Yonghui Li, Jiang Yang, Jianning Zhang, Xiaoyu Mu, Xiao-Dong Zhang","doi":"10.1016/j.cej.2025.159940","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159940","url":null,"abstract":"Biocatalytic activity of artificial nanozymes is strongly correlated with the detection sensitivity of lateral flow immunoassays (LFIA). Modulating the electronic structure is a promising and effective strategy to improve the catalytic activity of nanozymes, but remains a challenge. In this study, we develop a single-atom nanozyme LFIA platform with high active and electron-rich Pt single atoms onto AuPd support (Pt<sub>1</sub>/PA). The Pt<sub>1</sub>/PA nanozymes exhibit superior peroxidase (POD)-like activity with the catalytic efficiency (<em>K<sub>cat</sub>/K<sub>m</sub></em>) of 9.29 × 10<sup>6</sup> mM<sup>−1</sup>·min<sup>−1</sup>, which is 315-fold higher than natural horseradish peroxidase (HRP). Density Functional Theory calculations reveal that the remarkable activity is attributed to the formation of electron-rich site of Pt single atoms through electron transfer from support to Pt 5<em>d</em> orbitals, as well as <em>d</em>-band center modulation. Moreover, more electron transfer numbers are available for Pt single atoms at the surface in the lattice than outside the lattice. Benefiting from excellent biocatalytic activity, the limits of detection (LOD) of Pt<sub>1</sub>/PA-LFIA for carcinoembryonic antigen (CEA) and prostate-specific antigen (PSA) are 1.21pg mL<sup>−1</sup> and 0.6pg mL<sup>−1</sup>, which are 20.4 and 13.3-fold lower than commercial enzyme-linked immunosorbent assay kits (CEA: ab264604, 24.68pg mL<sup>−1</sup>; PSA: ab264615, 8pg mL<sup>−1</sup>), respectively. More importantly, Pt<sub>1</sub>/PA-LFIA achieves the accurate detection of prostate cancer and lung cancer clinical patients. This work presents a paradigm for ultrasensitive biomarker diagnostics based on single-atom nanozyme immunoassays.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"47 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044296","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The power conversion efficiency (PCE) of organic solar cells (OSCs) is intricately linked to the molecular design strategy of non-fullerene acceptors (NFAs). Researchers frequently modificated the end group and side chain in prior investigations. The central core of quinoxaline (Qx) possesses abundant modification sites, and the alkoxy groups exhibit high electron-accepting capability based on its meta-substitution. In this work, we designed and synthesized three small molecule acceptors (SMAs) with a phenyl substituted with an alkoxy group on their central core of quinoxaline, named Qx-B1, Qx-B2, and Qx-B3, respectively. The molecular backbones of these substances share similarities, yet the substitution points of methoxy groups are different, which significantly affect absorption, energy levels, electrostatic potentials, and molecular stacking of acceptors. As a result, the PM6:Qx-B2 device possessed excellent crystallinity and uniform morphology in the blend film, indicating outstanding charge transport and collection characteristics. This resulted in a high short-circuit current density (JSC) of 25.97 mA cm−2 and fill factor (FF) of 77.17 %, contributing to its champion PCE of 17.88 %. Furthermore, by using ternary and interface engineering strategies, when 15 wt% of BTP-eC9 was doped into the PM6:Qx-B2 two-component device as a guest acceptor, the 2PACz as the hole transparent layer, the device achieved a PCE of 19.25 %. This work investigates Qx-based asymmetric NFAs with three different methoxy substitution positions, suggesting a research direction for alkoxy substitution in the central core.
{"title":"Central core regulation by methoxy in quinoxaline-based non-fullerene acceptors for over 19% efficiency organic solar cells","authors":"Huijuan Bi, Dingding Qiu, Hao Zhang, Caixuan Wang, Mengying Wu, Xinya Ran, Jianqi Zhang, Yuheng Wang, Ailing Tang, Xinyang Miao, Zhixiang Wei, Kun Lu","doi":"10.1016/j.cej.2025.159972","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159972","url":null,"abstract":"The power conversion efficiency (PCE) of organic solar cells (OSCs) is intricately linked to the molecular design strategy of non-fullerene acceptors (NFAs). Researchers frequently modificated the end group and side chain in prior investigations. The central core of quinoxaline (Qx) possesses abundant modification sites, and the alkoxy groups exhibit high electron-accepting capability based on its <em>meta</em>-substitution. In this work, we designed and synthesized three small molecule acceptors (SMAs) with a phenyl substituted with an alkoxy group on their central core of quinoxaline, named Qx-B1, Qx-B2, and Qx-B3, respectively. The molecular backbones of these substances share similarities, yet the substitution points of methoxy groups are different, which significantly affect absorption, energy levels, electrostatic potentials, and molecular stacking of acceptors. As a result, the PM6:Qx-B2 device possessed excellent crystallinity and uniform morphology in the blend film, indicating outstanding charge transport and collection characteristics. This resulted in a high short-circuit current density (<em>J</em><sub>SC</sub>) of 25.97 mA cm<sup>−2</sup> and fill factor (FF) of 77.17 %, contributing to its champion PCE of 17.88 %. Furthermore, by using ternary and interface engineering strategies, when 15 wt% of BTP-eC9 was doped into the PM6:Qx-B2 two-component device as a guest acceptor, the 2PACz as the hole transparent layer, the device achieved a PCE of 19.25 %. This work investigates Qx-based asymmetric NFAs with three different methoxy substitution positions, suggesting a research direction for alkoxy substitution in the central core.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"206 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050778","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-27DOI: 10.1016/j.cej.2025.160011
Fengying Yi, Zeyu Li, Qingzhong Guo, Faliang Luo, Jiangyu Wu, Pu Hu, Zhihong Liu
The large-scale application of lithium metal batteries (LMBs) is restricted by the safety issues, particularly the flammablility of liquid electrolyte and the growth of lithium dendrites. Herein, a novel phosphorus-containing gel polymer electrolyte (GPE) was prepared in situ via thiol–ene click chemistry of ethyl di[2-(acryloyloxy) ethyl] phosphate and di- and tri-thiol monomers directly inside the battery. The GPEs exhibits exceptional flame retardancy and effectively reduces the risk of thermal runaway of batteries with GPE, maintaining high ionic conductivity of 1.42 × 10-3 S cm−1 at room temperature. The polymer skeleton contributes to the formation of inorganic/organic hybrid solid electrolyte interface (SEI) layer, which can effectively enhance interface stability and suppress the formation of lithium dendrites. As a results, the fabricated LiFePO4/GPE-3/Li cells exhibited excellent rate performance and stable cycling, retaining 90 % of capacity at 0.5C after 800 cycles. Furthermore, LiCoO2/GPE-3/Graphite full cells demonstrate a capacity retention of 95.7 % at 0.2C after 50 cycles within the voltage range of 3.0–4.45 V, confirming the superior cycling stability of GPE-3 in high-voltage, high-capacity battery systems. This work presents a GPE that not only enhances the safety of LMBs but also significantly improves their electrochemical performance, offering a promising solution for the practical application of high-energy–density LMBs.
{"title":"In situ preparation of nonflammable phosphorus-containing gel polymer electrolyte for lithium metal battery with enhanced interfacial stability and safety","authors":"Fengying Yi, Zeyu Li, Qingzhong Guo, Faliang Luo, Jiangyu Wu, Pu Hu, Zhihong Liu","doi":"10.1016/j.cej.2025.160011","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160011","url":null,"abstract":"The large-scale application of lithium metal batteries (LMBs) is restricted by the safety issues, particularly the flammablility of liquid electrolyte and the growth of lithium dendrites. Herein, a novel phosphorus-containing gel polymer electrolyte (GPE) was prepared in situ via thiol–ene click chemistry of ethyl di[2-(acryloyloxy) ethyl] phosphate and di- and tri-thiol monomers directly inside the battery. The GPEs exhibits exceptional flame retardancy and effectively reduces the risk of thermal runaway of batteries with GPE, maintaining high ionic conductivity of 1.42 × 10<sup>-3</sup> S cm<sup>−1</sup> at room temperature. The polymer skeleton contributes to the formation of inorganic/organic hybrid solid electrolyte interface (SEI) layer, which can effectively enhance interface stability and suppress the formation of lithium dendrites. As a results, the fabricated LiFePO<sub>4</sub>/GPE-3/Li cells exhibited excellent rate performance and stable cycling, retaining 90 % of capacity at 0.5C after 800 cycles. Furthermore, LiCoO<sub>2</sub>/GPE-3/Graphite full cells demonstrate a capacity retention of 95.7 % at 0.2C after 50 cycles within the voltage range of 3.0–4.45 V, confirming the superior cycling stability of GPE-3 in high-voltage, high-capacity battery systems. This work presents a GPE that not only enhances the safety of LMBs but also significantly improves their electrochemical performance, offering a promising solution for the practical application of high-energy–density LMBs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"24 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050783","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Layered vanadium-based materials are considered to be the most promising cathode materials for aqueous zinc ion batteries (AZIBs) due to their abundant valence changes and high theoretical capacity. However, low intrinsic conductivity, poor low temperature performance and generally poor cycle life hinder their further application. This study proposes a 3D conductive network by compositing vanadium-based materials with graphene to improve the conductivity for rapid electron transfer. Meanwhile, the interleaving of vanadium-based materials with the conductive network of graphene constructs a buffer layer, which can effectively mitigate the structural collapse caused by Zn2+ insertion/extraction during the charge and discharge processes, and significantly increase the long cycle life of the battery. The H2V3O8/rGO conductive network buffer layer is directly synthesized by a one-step hydrothermal method. The H2V3O8/rGO-100//Zn batteries show a specific capacity of up to 528.3 mAh/g at 0.1 A/g. Even at a high working current density of 20 A/g, the specific capacity is still 137.2 mAh/g, and it can remain 88.8 % after 12,000 cycles. Moreover, at the low temperature of −20 °C, the H2V3O8/rGO-100//Zn still maintain a high specific capacity of 346.6 mAh/g at 0.1 A/g, and its specific capacity can remain 86.2 % after 20,000 cycles at 10 A/g. Even at −30 °C, it can stably work for 3000 cycles at 1 A/g with almost no capacity degradation, showing good low temperature adaptability. Therefore, the present work provides a novelty strategy of designing cathode materials for ZIBs with excellent performance.
{"title":"Construction of three-dimensional conductive network layer by graphene and vanadium oxide composite for high performance long life low temperature aqueous zinc ion batteries","authors":"Ziwei Gan, Xiaohe Ren, Mingdong Liu, Nengze Wang, Tianning Pian, Mengxuan Sun, Chunyang Jia, Zhijie Li","doi":"10.1016/j.cej.2025.160013","DOIUrl":"https://doi.org/10.1016/j.cej.2025.160013","url":null,"abstract":"Layered vanadium-based materials are considered to be the most promising cathode materials for aqueous zinc ion batteries (AZIBs) due to their abundant valence changes and high theoretical capacity. However, low intrinsic conductivity, poor low temperature performance and generally poor cycle life hinder their further application. This study proposes a 3D conductive network by compositing vanadium-based materials with graphene to improve the conductivity for rapid electron transfer. Meanwhile, the interleaving of vanadium-based materials with the conductive network of graphene constructs a buffer layer, which can effectively mitigate the structural collapse caused by Zn<sup>2+</sup> insertion/extraction during the charge and discharge processes, and significantly increase the long cycle life of the battery. The H<sub>2</sub>V<sub>3</sub>O<sub>8</sub>/rGO conductive network buffer layer is directly synthesized by a one-step hydrothermal method. The H<sub>2</sub>V<sub>3</sub>O<sub>8</sub>/rGO-100//Zn batteries show a specific capacity of up to 528.3 mAh/g at 0.1 A/g. Even at a high working current density of 20 A/g, the specific capacity is still 137.2 mAh/g, and it can remain 88.8 % after 12,000 cycles. Moreover, at the low temperature of −20 °C, the H<sub>2</sub>V<sub>3</sub>O<sub>8</sub>/rGO-100//Zn still maintain a high specific capacity of 346.6 mAh/g at 0.1 A/g, and its specific capacity can remain 86.2 % after 20,000 cycles at 10 A/g. Even at −30 °C, it can stably work for 3000 cycles at 1 A/g with almost no capacity degradation, showing good low temperature adaptability. Therefore, the present work provides a novelty strategy of designing cathode materials for ZIBs with excellent performance.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"35 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050787","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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