Pub Date : 2024-11-14DOI: 10.1016/j.cej.2024.157387
Jia Wang, Shuangrong Wu, Ke Liu, Qi Yang, Haoze Liu, Zhilin Yang
Overconsumption in industrial manufacturing has led to critical emissions of chloroalkanes, posing a significant environmental threat. In this study, the innovative biochar (BC) particles containing nanocrystalline: NZVI, Fe/Pd, Fe/Ni were prepared by impregnation-liquid phase reduction using the pyrolysis of coconut husk as precursors to explore the degradation capabilities of chloroform (CF) via orthogonal experiment. The results indicated that when the pH value was 3, the temperature was 20 ℃, and the reaction time was 60 min, the CF removal efficiency of Fe/Ni-BC reached 80.38 ± 2.08 %, outperforming all other tested synthetic particles. Advanced characterization techniques showed that the abundant dispersed metallic nanoparticle sites would refresh the surface crystal morphology, improve the adsorption enrichment ability of biochar, enhance electron transfer capacity of synthetic particles, and further participate in reductive dechlorination by inducing an electrophilic attack of active hydrogen. Theoretical calculations verified that hydrogen activation and CF facile adsorption would be easily achieved after the introduction of metal nanoparticles, profiting from the multiple synergistic effects between special π-delocalized bond of biochar in carbon layer and multiple nanoparticles docking sites, and thus enhancing the specific CF catalytic selectivity of Fe/Ni as the active center. Collectively, the CF degradation on Fe/Ni-BC was a complex chemisorption process along with reductive hydrogenation decomposition, which achieved the parent CF reduction and promoted the conversion of the low-chlorinated benign products. These findings offer new insights into the developed multifunctional BC and their comprehensive assessment of CF sewage remediation.
{"title":"The investigation of highly efficient chlorinated hydrocarbons removal based on metal nanoparticles carbonaceous synthetic particles: The degradation behavior and selective transformation mechanism","authors":"Jia Wang, Shuangrong Wu, Ke Liu, Qi Yang, Haoze Liu, Zhilin Yang","doi":"10.1016/j.cej.2024.157387","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157387","url":null,"abstract":"Overconsumption in industrial manufacturing has led to critical emissions of chloroalkanes, posing a significant environmental threat. In this study, the innovative biochar (BC) particles containing nanocrystalline: NZVI, Fe/Pd, Fe/Ni were prepared by impregnation-liquid phase reduction using the pyrolysis of coconut husk as precursors to explore the degradation capabilities of chloroform (CF) via orthogonal experiment. The results indicated that when the pH value was 3, the temperature was 20 ℃, and the reaction time was 60 min, the CF removal efficiency of Fe/Ni-BC reached 80.38 ± 2.08 %, outperforming all other tested synthetic particles. Advanced characterization techniques showed that the abundant dispersed metallic nanoparticle sites would refresh the surface crystal morphology, improve the adsorption enrichment ability of biochar, enhance electron transfer capacity of synthetic particles, and further participate in reductive dechlorination by inducing an electrophilic attack of active hydrogen. Theoretical calculations verified that hydrogen activation and CF facile adsorption would be easily achieved after the introduction of metal nanoparticles, profiting from the multiple synergistic effects between special π-delocalized bond of biochar in carbon layer and multiple nanoparticles docking sites, and thus enhancing the specific CF catalytic selectivity of Fe/Ni as the active center. Collectively, the CF degradation on Fe/Ni-BC was a complex chemisorption process along with reductive hydrogenation decomposition, which achieved the parent CF reduction and promoted the conversion of the low-chlorinated benign products. These findings offer new insights into the developed multifunctional BC and their comprehensive assessment of CF sewage remediation.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"14 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610393","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Joanna Su Xian Chong, Fang Ji, Saima Hilal, Joyce Ruifen Chong, Jia Ming Lau, Nathanael Ren Jie Tong, Boon Yeow Tan, Narayanaswamy Venketasubramanian, Mitchell Kim Peng Lai, Christopher Li‐Hsian Chen, Juan Helen Zhou
INTRODUCTIONWe investigated the effects of multiple cerebrovascular disease (CeVD) neuroimaging markers on brain functional connectivity (FC), and how such CeVD‐related FC changes interact with plasma phosphorylated tau (p‐tau)181 (an Alzheimer's disease [AD] marker) to influence downstream neurodegeneration and cognitive changes.METHODSMultivariate associations among four CeVD markers and whole‐brain FC in 529 participants across the dementia spectrum were examined using partial least squares correlation. Interactive effects of CeVD‐related FC patterns and p‐tau181 on longitudinal gray matter volume (GMV) and cognitive changes were investigated using linear mixed‐effects models.RESULTSWe identified a brain FC phenotype associated with high CeVD burden across all markers. Further, expression of this general CeVD‐related FC phenotype and p‐tau181 contributed additively, but not synergistically, to baseline and longitudinal GMV and cognitive changes.DISCUSSIONOur findings suggest that CeVD exerts global effects on the brain connectome and highlight the additive nature of AD and CeVD on neurodegeneration and cognition.HighlightsEffects of multiple cerebrovascular disease (CeVD) markers on functional connectivity were studied.A global network phenotype linked to high burden across CeVD markers was identified.CeVD phenotype and plasma phosphorylated tau 181 contributed additively to downstream outcomes.
引言我们研究了多种脑血管疾病（CeVD）神经影像学标志物对大脑功能连接性（FC）的影响，以及这种与CeVD相关的FC变化如何与血浆磷酸化tau（p-tau）181（一种阿尔茨海默病[AD]标志物）相互作用，从而影响下游神经变性和认知变化.方法使用偏最小二乘法相关性检验了痴呆症谱系中529名参与者的四种CeVD标志物与全脑FC之间的多变量关联。使用线性混合效应模型研究了CeVD相关FC模式和p-tau181对纵向灰质体积（GMV）和认知变化的交互影响。讨论我们的研究结果表明，CeVD 对大脑连接组产生了整体影响，并强调了 AD 和 CeVD 对神经退化和认知的叠加作用。研究发现了一种与高负担CeVD标记物相关的全球网络表型。CeVD表型和血浆磷酸化tau 181对下游结果的影响是叠加的。
{"title":"Additive effects of cerebrovascular disease functional connectome phenotype and plasma p‐tau181 on longitudinal neurodegeneration and cognitive outcomes","authors":"Joanna Su Xian Chong, Fang Ji, Saima Hilal, Joyce Ruifen Chong, Jia Ming Lau, Nathanael Ren Jie Tong, Boon Yeow Tan, Narayanaswamy Venketasubramanian, Mitchell Kim Peng Lai, Christopher Li‐Hsian Chen, Juan Helen Zhou","doi":"10.1002/alz.14328","DOIUrl":"https://doi.org/10.1002/alz.14328","url":null,"abstract":"INTRODUCTIONWe investigated the effects of multiple cerebrovascular disease (CeVD) neuroimaging markers on brain functional connectivity (FC), and how such CeVD‐related FC changes interact with plasma phosphorylated tau (p‐tau)181 (an Alzheimer's disease [AD] marker) to influence downstream neurodegeneration and cognitive changes.METHODSMultivariate associations among four CeVD markers and whole‐brain FC in 529 participants across the dementia spectrum were examined using partial least squares correlation. Interactive effects of CeVD‐related FC patterns and p‐tau181 on longitudinal gray matter volume (GMV) and cognitive changes were investigated using linear mixed‐effects models.RESULTSWe identified a brain FC phenotype associated with high CeVD burden across all markers. Further, expression of this general CeVD‐related FC phenotype and p‐tau181 contributed additively, but not synergistically, to baseline and longitudinal GMV and cognitive changes.DISCUSSIONOur findings suggest that CeVD exerts global effects on the brain connectome and highlight the additive nature of AD and CeVD on neurodegeneration and cognition.Highlights<jats:list list-type=\"bullet\"> <jats:list-item>Effects of multiple cerebrovascular disease (CeVD) markers on functional connectivity were studied.</jats:list-item> <jats:list-item>A global network phenotype linked to high burden across CeVD markers was identified.</jats:list-item> <jats:list-item>CeVD phenotype and plasma phosphorylated tau 181 contributed additively to downstream outcomes.</jats:list-item> </jats:list>","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"98 1","pages":""},"PeriodicalIF":14.0,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610401","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-14DOI: 10.1016/j.cej.2024.157638
Jiahao Du, Haozhen Li, Jinhua Zhang, Wenhao Wang, Zhen Li, Qingchan Li, Jinxiang Li
There is a trade-off between corrosion and decontamination of nanoscale zero-valent iron (nZVI), which can be modulated by the sulfidation. Despite that, the insights into the relationship between anaerobic corrosion and decontamination of sulfidated nZVI (S-nZVI) remain unclear from a kinetic point of view. Herein, we used the variation of open-circuit potential to explore the anaerobic corrosion kinetic of S-nZVI. Taking Cr(VI) as the targeted contaminant, a negative correlation between decontamination and the corrosion of S-nZVI was identified during the first 10 min of reaction (R2 = 0.6919, slope = -0.7091) and after the 10 min of reaction (R2 = 0.7556, slope = -0.1307). Based on the results of TEM mapping, electrochemical impedance spectroscopy and XPS, this study further revealed that sulfidation not only enhanced the mass transfer of Cr(VI) toward nZVI in the initial stage of reaction, but also improved the electron transfer of nZVI toward Cr(VI) in the later stage of reaction. The ultimately enhanced removal and reduction of Cr(VI) by S-nZVI should be attributed to the introduction of iron sulfides (FeSx) that not only promoted the conductivity but also favored the affinity of nZVI toward Cr(VI). Overall, the kinetic insights presented in this study are valuable for understanding the process mechanisms of S-nZVI in anaerobic water and may extend to provide theoretical support for the development of enhanced methods for the remediation of contaminated groundwater using nZVI.
{"title":"Kinetic insights into the relationships between anaerobic corrosion and decontamination of nanoscale zerovalent iron improved by sulfidation","authors":"Jiahao Du, Haozhen Li, Jinhua Zhang, Wenhao Wang, Zhen Li, Qingchan Li, Jinxiang Li","doi":"10.1016/j.cej.2024.157638","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157638","url":null,"abstract":"There is a trade-off between corrosion and decontamination of nanoscale zero-valent iron (nZVI), which can be modulated by the sulfidation. Despite that, the insights into the relationship between anaerobic corrosion and decontamination of sulfidated nZVI (S-nZVI) remain unclear from a kinetic point of view. Herein, we used the variation of open-circuit potential to explore the anaerobic corrosion kinetic of S-nZVI. Taking Cr(VI) as the targeted contaminant, a negative correlation between decontamination and the corrosion of S-nZVI was identified during the first 10 min of reaction (R<sup>2</sup> = 0.6919, slope = -0.7091) and after the 10 min of reaction (R<sup>2</sup> = 0.7556, slope = -0.1307). Based on the results of TEM mapping, electrochemical impedance spectroscopy and XPS, this study further revealed that sulfidation not only enhanced the mass transfer of Cr(VI) toward nZVI in the initial stage of reaction, but also improved the electron transfer of nZVI toward Cr(VI) in the later stage of reaction. The ultimately enhanced removal and reduction of Cr(VI) by S-nZVI should be attributed to the introduction of iron sulfides (FeS<sub>x</sub>) that not only promoted the conductivity but also favored the affinity of nZVI toward Cr(VI). Overall, the kinetic insights presented in this study are valuable for understanding the process mechanisms of S-nZVI in anaerobic water and may extend to provide theoretical support for the development of enhanced methods for the remediation of contaminated groundwater using nZVI.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"20 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610282","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In semiconductor catalysts, long-lived excited states can effectually improve the utilization of photogenerated carriers to enhance photocatalytic performance. Herein, we used supramolecular engineering to synthesize a hollow tubular carbon nitride catalyst with N vacancies and an obvious n–π* transition. The unique hollow tubular structure provides abundant active sites, which are favorable for photocatalytic reaction. The presence of N vacancies expands the π-electron delocalization domains in the conjugated system, which excites the n–π* transition and thus triggers the red-shifted absorption edge at approximately 660 nm. Experiments and DFT calculations demonstrated that the N vacancies are beneficial for narrowing the bandgap and promoting the reduction of H+ by photogenerated electrons. Femtosecond transient absorption spectroscopy (fs-TAS) indicated that the n–π* electronic transition in the carbon nitride photocatalyst leads to slower exciton annihilation (lifetime: 38.64 ± 10.6 ps) and extended shallow electron trapping states (lifetime: 325.9 ± 19.3 ps). The appearance of these states adds more photogenerated electrons to the photocatalytic reaction process. The optimal hollow tubular carbon nitride catalyst exhibits a hydrogen production rate of 2664.47 μmol∙g−1∙h−1, which is 31.2 times higher than that of bulk carbon nitride (85.3325 μmol∙g−1∙h−1). This work highlights the ability of the n–π* transition induced by N vacancies to enhance the photocatalytic activity of carbon nitride.
{"title":"The n–π* electronic transition induced by nitrogen vacancies enhances photocatalytic hydrogen production in carbon nitride","authors":"Zhili Xu, Jing Li, Deyi Zhan, Yue Liu, Weihong Xu, Junfeng Wang, Zhiwu Yu","doi":"10.1016/j.cej.2024.157670","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157670","url":null,"abstract":"In semiconductor catalysts, long-lived excited states can effectually improve the utilization of photogenerated carriers to enhance photocatalytic performance. Herein, we used supramolecular engineering to synthesize a hollow tubular carbon nitride catalyst with N vacancies and an obvious n–π* transition. The unique hollow tubular structure provides abundant active sites, which are favorable for photocatalytic reaction. The presence of N vacancies expands the π-electron delocalization domains in the conjugated system, which excites the n–π* transition and thus triggers the red-shifted absorption edge at approximately 660 nm. Experiments and DFT calculations demonstrated that the N vacancies are beneficial for narrowing the bandgap and promoting the reduction of H<sup>+</sup> by photogenerated electrons. Femtosecond transient absorption spectroscopy (fs-TAS) indicated that the n–π* electronic transition in the carbon nitride photocatalyst leads to slower exciton annihilation (lifetime: 38.64 ± 10.6 ps) and extended shallow electron trapping states (lifetime: 325.9 ± 19.3 ps). The appearance of these states adds more photogenerated electrons to the photocatalytic reaction process. The optimal hollow tubular carbon nitride catalyst exhibits a hydrogen production rate of 2664.47 μmol∙g<sup>−1</sup>∙h<sup>−1</sup>, which is 31.2 times higher than that of bulk carbon nitride (85.3325 μmol∙g<sup>−1</sup>∙h<sup>−1</sup>). This work highlights the ability of the n–π* transition induced by N vacancies to enhance the photocatalytic activity of carbon nitride.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"5 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610283","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-14DOI: 10.1016/j.cej.2024.157462
Timan Lei, Junyu Yang, Geng Wang, Jin Chen, Yinglong He, Kai H. Luo
Non-aqueous Li–<span><span><math><msub is="true"><mrow is="true"><mtext is="true">O</mtext></mrow><mrow is="true"><mn is="true">2</mn></mrow></msub></math></span><script type="math/mml"><math><msub is="true"><mrow is="true"><mtext is="true">O</mtext></mrow><mrow is="true"><mn is="true">2</mn></mrow></msub></math></script></span> battery (NALiO2B) is a promising alternative to lithium-ion batteries, offering high theoretical energy density. However, its practical applications are hampered by limited understanding of the underlying mechanisms. In this study, a three-dimensional electrochemical lattice Boltzmann method is proposed to simulate the physical and electrochemical processes during NALiO2B discharge at the pore scale. The discharge performance of NALiO2B is evaluated for various electrode and electrolyte designs. It is found that the limited <span><span><math><msub is="true"><mrow is="true"><mtext is="true">O</mtext></mrow><mrow is="true"><mn is="true">2</mn></mrow></msub></math></span><script type="math/mml"><math><msub is="true"><mrow is="true"><mtext is="true">O</mtext></mrow><mrow is="true"><mn is="true">2</mn></mrow></msub></math></script></span> diffusion within homogeneous electrodes is the primary cause of the declined reactive electrode surface area, the intensified electrochemical reaction (or overpotential), and finally the premature battery death. This issue can be mitigated by employing the hierarchical electrode <span><span><math><msub is="true"><mrow is="true"><mtext is="true">BP</mtext></mrow><mrow is="true"><mn is="true">2</mn></mrow></msub></math></span><script type="math/mml"><math><msub is="true"><mrow is="true"><mtext is="true">BP</mtext></mrow><mrow is="true"><mn is="true">2</mn></mrow></msub></math></script></span> with a bi-porous structure. The large pores in <span><span><math><msub is="true"><mrow is="true"><mtext is="true">BP</mtext></mrow><mrow is="true"><mn is="true">2</mn></mrow></msub></math></span><script type="math/mml"><math><msub is="true"><mrow is="true"><mtext is="true">BP</mtext></mrow><mrow is="true"><mn is="true">2</mn></mrow></msub></math></script></span> improve <span><span><math><msub is="true"><mrow is="true"><mtext is="true">O</mtext></mrow><mrow is="true"><mn is="true">2</mn></mrow></msub></math></span><script type="math/mml"><math><msub is="true"><mrow is="true"><mtext is="true">O</mtext></mrow><mrow is="true"><mn is="true">2</mn></mrow></msub></math></script></span> transport to sustain the stable reaction process, thus enhancing the discharge capacity of NALiO2B. To further boost the rate capability of NALiO2B, <span><span><math><msub is="true"><mrow is="true"><mtext is="true">BP</mtext></mrow><mrow is="true"><mn is="true">2</mn></mrow></msub></math></span><script type="math/mml"><math><msub is="true"><mrow is="true"><mtext is="true">BP</mtext></mrow><mrow is="true"><mn is="true">2</mn></mrow></msub></math></script></span> is partially infiltrated with electrolyte to form the multiphase (MP)
{"title":"Insight into discharge of non-aqueous Li–O2 battery using a three-dimensional electrochemical lattice Boltzmann model","authors":"Timan Lei, Junyu Yang, Geng Wang, Jin Chen, Yinglong He, Kai H. Luo","doi":"10.1016/j.cej.2024.157462","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157462","url":null,"abstract":"Non-aqueous Li–<span><span><math><msub is=\"true\"><mrow is=\"true\"><mtext is=\"true\">O</mtext></mrow><mrow is=\"true\"><mn is=\"true\">2</mn></mrow></msub></math></span><script type=\"math/mml\"><math><msub is=\"true\"><mrow is=\"true\"><mtext is=\"true\">O</mtext></mrow><mrow is=\"true\"><mn is=\"true\">2</mn></mrow></msub></math></script></span> battery (NALiO2B) is a promising alternative to lithium-ion batteries, offering high theoretical energy density. However, its practical applications are hampered by limited understanding of the underlying mechanisms. In this study, a three-dimensional electrochemical lattice Boltzmann method is proposed to simulate the physical and electrochemical processes during NALiO2B discharge at the pore scale. The discharge performance of NALiO2B is evaluated for various electrode and electrolyte designs. It is found that the limited <span><span><math><msub is=\"true\"><mrow is=\"true\"><mtext is=\"true\">O</mtext></mrow><mrow is=\"true\"><mn is=\"true\">2</mn></mrow></msub></math></span><script type=\"math/mml\"><math><msub is=\"true\"><mrow is=\"true\"><mtext is=\"true\">O</mtext></mrow><mrow is=\"true\"><mn is=\"true\">2</mn></mrow></msub></math></script></span> diffusion within homogeneous electrodes is the primary cause of the declined reactive electrode surface area, the intensified electrochemical reaction (or overpotential), and finally the premature battery death. This issue can be mitigated by employing the hierarchical electrode <span><span><math><msub is=\"true\"><mrow is=\"true\"><mtext is=\"true\">BP</mtext></mrow><mrow is=\"true\"><mn is=\"true\">2</mn></mrow></msub></math></span><script type=\"math/mml\"><math><msub is=\"true\"><mrow is=\"true\"><mtext is=\"true\">BP</mtext></mrow><mrow is=\"true\"><mn is=\"true\">2</mn></mrow></msub></math></script></span> with a bi-porous structure. The large pores in <span><span><math><msub is=\"true\"><mrow is=\"true\"><mtext is=\"true\">BP</mtext></mrow><mrow is=\"true\"><mn is=\"true\">2</mn></mrow></msub></math></span><script type=\"math/mml\"><math><msub is=\"true\"><mrow is=\"true\"><mtext is=\"true\">BP</mtext></mrow><mrow is=\"true\"><mn is=\"true\">2</mn></mrow></msub></math></script></span> improve <span><span><math><msub is=\"true\"><mrow is=\"true\"><mtext is=\"true\">O</mtext></mrow><mrow is=\"true\"><mn is=\"true\">2</mn></mrow></msub></math></span><script type=\"math/mml\"><math><msub is=\"true\"><mrow is=\"true\"><mtext is=\"true\">O</mtext></mrow><mrow is=\"true\"><mn is=\"true\">2</mn></mrow></msub></math></script></span> transport to sustain the stable reaction process, thus enhancing the discharge capacity of NALiO2B. To further boost the rate capability of NALiO2B, <span><span><math><msub is=\"true\"><mrow is=\"true\"><mtext is=\"true\">BP</mtext></mrow><mrow is=\"true\"><mn is=\"true\">2</mn></mrow></msub></math></span><script type=\"math/mml\"><math><msub is=\"true\"><mrow is=\"true\"><mtext is=\"true\">BP</mtext></mrow><mrow is=\"true\"><mn is=\"true\">2</mn></mrow></msub></math></script></span> is partially infiltrated with electrolyte to form the multiphase (MP)","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"11 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610289","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-14DOI: 10.1016/j.cej.2024.157685
Stefan Desimpel, Jan Dijkmans, Koen P.L. Kuijpers, Matthieu Dorbec, Kevin M. Van Geem, Christian V. Stevens
We developed an automated platform capable of performing photochemical gas–liquid reactions. The platform was augmented with a state-of-the-art Bayesian optimization algorithm and was tested on the decatungstate-catalyzed aerobic oxidation of ethyl benzene, to optimize both yield and productivity, and identify the Pareto front of these objectives. Although photochemical gas–liquid systems are highly complex due to numerous interactions between the parameters, including effects on mass-transfer, gas solubility and light absorption, the algorithm demonstrated impressive speed to navigate the parameter space towards optimal conditions. Furthermore, this approach also proved highly flexible, allowing for modification of objectives and parameter ranges on the fly. The identified conditions were then tested on a select scope of substrates, to better understand the generality of these conditions, especially on molecules where selectivity comes into play. The results show the platform to be a useful tool for reaction optimization and process intensification.
{"title":"Efficient multi-objective Bayesian optimization of gas–liquid photochemical reactions using an automated flow platform","authors":"Stefan Desimpel, Jan Dijkmans, Koen P.L. Kuijpers, Matthieu Dorbec, Kevin M. Van Geem, Christian V. Stevens","doi":"10.1016/j.cej.2024.157685","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157685","url":null,"abstract":"We developed an automated platform capable of performing photochemical gas–liquid reactions. The platform was augmented with a state-of-the-art Bayesian optimization algorithm and was tested on the decatungstate-catalyzed aerobic oxidation of ethyl benzene, to optimize both yield and productivity, and identify the Pareto front of these objectives. Although photochemical gas–liquid systems are highly complex due to numerous interactions between the parameters, including effects on mass-transfer, gas solubility and light absorption, the algorithm demonstrated impressive speed to navigate the parameter space towards optimal conditions. Furthermore, this approach also proved highly flexible, allowing for modification of objectives and parameter ranges on the fly. The identified conditions were then tested on a select scope of substrates, to better understand the generality of these conditions, especially on molecules where selectivity comes into play. The results show the platform to be a useful tool for reaction optimization and process intensification.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"6 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609830","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-14DOI: 10.1016/j.cej.2024.157266
Huadong Gao, Yang Xiong, Bo Rui, Yinhua Bao, Yicheng Song, Bo Lu, Junqian Zhang
Inspired by chocolate patterning, this paper proposes a facile mechanical imprinting method for constructing novel flexible thick electrodes in response to the rapid development of multifunctional batteries. Appropriately designed imprinting of the active layer in a semi-dry state during the drying process can introduce stable ridge-slot patterns within the thick electrodes, which requires only low-cost and scalable templates with minimal modifications to the electrode fabrication process. Due to imprinting introducing ion transport channels in the electrode thickness direction, electrochemical cycling performance of imprinted thick electrodes can be significantly enhanced compared to conventional thick electrodes. For high C-rate conditions, the areal capacity of the thick electrode can be increased by up to approximately 225 % due to the imprinting, while the cycling remains stable. More interestingly, these thick electrodes with ridge-slot patterns exhibit remarkable flexibility due to the fact that the slot portion acts as a “joint”. The capacity loss of a pouch cell containing the imprinted electrode loses only about 4 % of its capacity after 10,000 bending cycles. Based on these results, this work provides a novel pathway for the development of flexible thick electrodes for multifunctional high-capacity batteries.
受巧克力图案的启发，本文提出了一种简便的机械压印方法，用于构建新型柔性厚电极，以应对多功能电池的快速发展。在干燥过程中，对处于半干状态的活性层进行适当的压印设计，可在厚电极中引入稳定的脊槽图案，这只需要低成本和可扩展的模板，对电极制造工艺的改动极小。由于压印在电极厚度方向上引入了离子传输通道，与传统的厚电极相比，压印厚电极的电化学循环性能可显著提高。在高 C 速率条件下，由于压印作用，厚电极的面积容量最多可增加约 225%，同时循环性能保持稳定。更有趣的是，这些带有脊槽图案的厚电极具有显著的柔韧性，这是因为槽的部分起到了 "连接 "的作用。含有压印电极的袋式电池在经过 10,000 次弯曲循环后，容量损失仅为原来的 4%。基于这些结果，这项研究为多功能高容量电池柔性厚电极的开发提供了一条新途径。
{"title":"Chocolate pattern-inspired flexible thick electrodes: A facile mechanical imprinting method","authors":"Huadong Gao, Yang Xiong, Bo Rui, Yinhua Bao, Yicheng Song, Bo Lu, Junqian Zhang","doi":"10.1016/j.cej.2024.157266","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157266","url":null,"abstract":"Inspired by chocolate patterning, this paper proposes a facile mechanical imprinting method for constructing novel flexible thick electrodes in response to the rapid development of multifunctional batteries. Appropriately designed imprinting of the active layer in a semi-dry state during the drying process can introduce stable ridge-slot patterns within the thick electrodes, which requires only low-cost and scalable templates with minimal modifications to the electrode fabrication process. Due to imprinting introducing ion transport channels in the electrode thickness direction, electrochemical cycling performance of imprinted thick electrodes can be significantly enhanced compared to conventional thick electrodes. For high C-rate conditions, the areal capacity of the thick electrode can be increased by up to approximately 225 % due to the imprinting, while the cycling remains stable. More interestingly, these thick electrodes with ridge-slot patterns exhibit remarkable flexibility due to the fact that the slot portion acts as a “joint”. The capacity loss of a pouch cell containing the imprinted electrode loses only about 4 % of its capacity after 10,000 bending cycles. Based on these results, this work provides a novel pathway for the development of flexible thick electrodes for multifunctional high-capacity batteries.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"46 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610334","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The utilization of renewable, non–edible biomass for synthesis of valuable bio–products, such as bio–fuels, and bio–polymeric materials, in an environmentally sustainable manner is crucial for addressing the urgent environmental challenges caused by our substantial dependence on fossil fuel resources. In this context, engineered microbial cell factories (MCFs), which are modified microorganisms, have gained attention and mainly involve biosynthetically optimized pathways for the production of desired bio–commodities using renewable carbon sources. Biosynthetic routes for the production of such bio–commodities can be categorized into three groups based on the chosen microbial host for genetic modification: native, non–native, and artificially produced pathways. Engineered MCFs are increasingly essential in the pharmaceutical, food, and bio–chemical industries and are being developed to address the growing world population and socioeconomic crisis. Mainly, microorganisms have been utilized in the manufacture of a range of bio–products, such as amino acids, carboxylic acids, carotenoids, enzymes, vitamins, plant natural products, biogas, and other biofuels. Furthermore, the implementation of metabolic engineering techniques enhances the speed, concentration, and efficiency of commercially important substances by modifying the carbon–energy balance and eliminating an undesired ATP sink, metabolism, physiology, and stress response. Industrial biotechnology is experiencing rapid growth due to engineered MCFs for production of several bio–commodities. This review summarizes the design of MFCs, selection of microbial strains, metabolic pathways, engineered MCFs for industrial–scale applications, strategies for engineering microbial robustness, commercial restrictions, and their future prospects.
以环境可持续的方式利用可再生的非食用生物质合成有价值的生物产品，如生物燃料和生物聚合材料，对于应对因严重依赖化石燃料资源而造成的紧迫环境挑战至关重要。在此背景下，工程微生物细胞工厂（MCFs）（一种改良微生物）受到关注，主要涉及利用可再生碳源生产所需生物商品的生物合成优化途径。根据所选择的基因修饰微生物宿主，生产此类生物商品的生物合成途径可分为三类：本地途径、非本地途径和人工途径。工程微生物菌群在制药、食品和生物化学工业中越来越重要，目前正在开发这种菌群，以应对不断增长的世界人口和社会经济危机。主要是利用微生物制造一系列生物产品，如氨基酸、羧酸、类胡萝卜素、酶、维生素、植物天然产品、沼气和其他生物燃料。此外，新陈代谢工程技术通过改变碳-能量平衡和消除不需要的 ATP 吸收汇、新陈代谢、生理和应激反应，提高了商业上重要物质的生产速度、浓度和效率。工业生物技术的快速发展得益于用于生产多种生物商品的工程化 MCF。本综述概述了 MFC 的设计、微生物菌株的选择、代谢途径、用于工业规模应用的工程 MCF、微生物稳健性工程策略、商业限制及其未来前景。
{"title":"Industrial–scale production of various bio–commodities by engineered MCFs: Strategies of engineering in microbial robustness","authors":"Ju-Hyeong Jung, Vinoth Kumar Ponnusamy, Gopalakrishnan Kumar, Bartłomiej Igliński, Vinod Kumar, Gergorz Piechota","doi":"10.1016/j.cej.2024.157679","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157679","url":null,"abstract":"The utilization of renewable, non–edible biomass for synthesis of valuable bio–products, such as bio–fuels, and bio–polymeric materials, in an environmentally sustainable manner is crucial for addressing the urgent environmental challenges caused by our substantial dependence on fossil fuel resources. In this context, engineered microbial cell factories (MCFs), which are modified microorganisms, have gained attention and mainly involve biosynthetically optimized pathways for the production of desired bio–commodities using renewable carbon sources. Biosynthetic routes for the production of such bio–commodities can be categorized into three groups based on the chosen microbial host for genetic modification: native, non–native, and artificially produced pathways. Engineered MCFs are increasingly essential in the pharmaceutical, food, and bio–chemical industries and are being developed to address the growing world population and socioeconomic crisis. Mainly, microorganisms have been utilized in the manufacture of a range of bio–products, such as amino acids, carboxylic acids, carotenoids, enzymes, vitamins, plant natural products, biogas, and other biofuels. Furthermore, the implementation of metabolic engineering techniques enhances the speed, concentration, and efficiency of commercially important substances by modifying the carbon–energy balance and eliminating an undesired ATP sink, metabolism, physiology, and stress response. Industrial biotechnology is experiencing rapid growth due to engineered MCFs for production of several bio–commodities. This review summarizes the design of MFCs, selection of microbial strains, metabolic pathways, engineered MCFs for industrial–scale applications, strategies for engineering microbial robustness, commercial restrictions, and their future prospects.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"34 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610285","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-14DOI: 10.1016/j.cej.2024.157477
Gansu Zhang, Hongyang Li, Zhiqiang Li, Shuxian Su, Xuan Xu, Liang Dong, Wei Dai, Qinglai Wei
Evolutionary identification of hydrodynamics from pressure signals is crucial for advancing the precise control of dry coal separation. Dynamic Mode Decomposition (DMD) is the key method to construct the data-driven control framework. Pressure signals rather than snapshots are investigated for industrial applications, bringing challenges to the implementation of DMD. The techniques of time delay embedding and optimal amplitude are introduced to make DMD work better for pressure signals. Comprehensive parameter tests of stack dimension and truncation order are carried out to seek for optimal identification performance. Due to parameter sensitivity, the qualification verification by sliding windows is performed to determine the robustness of parameter pairs. Spatiotemporal coherent structures are extracted to guide the regulation of separation process. In order to avoid the inefficiency of control, a heuristic sparsity promoting method using pruning is proposed to obtain a reduced order model. The original modes more than 100 can be reduced to approximately 35 primary modes. Furthermore, the Prune dominant frequency is defined, which can perceive the subtle fluctuations of temporal evolution than FFT and DMD for the long-term time. Present study provides the insight of hydrodynamics of dense gas-solid fluidized bed, establishing the foundation for future control studies of dry coal separation.
{"title":"Evolutionary identification in dense separation fluidized beds using dynamic mode decomposition with pruning","authors":"Gansu Zhang, Hongyang Li, Zhiqiang Li, Shuxian Su, Xuan Xu, Liang Dong, Wei Dai, Qinglai Wei","doi":"10.1016/j.cej.2024.157477","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157477","url":null,"abstract":"Evolutionary identification of hydrodynamics from pressure signals is crucial for advancing the precise control of dry coal separation. Dynamic Mode Decomposition (DMD) is the key method to construct the data-driven control framework. Pressure signals rather than snapshots are investigated for industrial applications, bringing challenges to the implementation of DMD. The techniques of time delay embedding and optimal amplitude are introduced to make DMD work better for pressure signals. Comprehensive parameter tests of stack dimension <span><span style=\"\"></span><span data-mathml='<math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mi is=\"true\">s</mi></math>' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"><svg aria-hidden=\"true\" focusable=\"false\" height=\"1.394ex\" role=\"img\" style=\"vertical-align: -0.235ex;\" viewbox=\"0 -498.8 469.5 600.2\" width=\"1.09ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"><g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"><g is=\"true\"><use xlink:href=\"#MJMATHI-73\"></use></g></g></svg><span role=\"presentation\"><math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mi is=\"true\">s</mi></math></span></span><script type=\"math/mml\"><math><mi is=\"true\">s</mi></math></script></span> and truncation order <span><span style=\"\"></span><span data-mathml='<math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mi is=\"true\">r</mi></math>' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"><svg aria-hidden=\"true\" focusable=\"false\" height=\"1.394ex\" role=\"img\" style=\"vertical-align: -0.235ex;\" viewbox=\"0 -498.8 451.5 600.2\" width=\"1.049ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"><g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"><g is=\"true\"><use xlink:href=\"#MJMATHI-72\"></use></g></g></svg><span role=\"presentation\"><math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mi is=\"true\">r</mi></math></span></span><script type=\"math/mml\"><math><mi is=\"true\">r</mi></math></script></span> are carried out to seek for optimal identification performance. Due to parameter sensitivity, the qualification verification by sliding windows is performed to determine the robustness of parameter pairs. Spatiotemporal coherent structures are extracted to guide the regulation of separation process. In order to avoid the inefficiency of control, a heuristic sparsity promoting method using pruning is proposed to obtain a reduced order model. The original modes more than 100 can be reduced to approximately 35 primary modes. Furthermore, the Prune dominant frequency is defined, which can perceive the subtle fluctuations of temporal evolution than FFT and DMD for the long-term time. Present study provides the insight of hydrodynamics of dense gas-solid fluidized bed, establishing the foundation for future control studies of dry coal separation.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"25 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610332","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Utilizing neural tissue engineering scaffolds to improve and reconstruct the injury microenvironment has shown great promise for repairing spinal cord injury (SCI). Here, we present a type of magnetic nanochain-induced anisotropic nerve assembly for SCI repair. Under the magnetical drive, silica-coated magnetic nanoparticles assemble into highly stable nanochains, further integrated into the hydrogel and controlled by a magnetic field to form an anisotropic array in a three-dimensional space. In vitro studies confirm that the prepared anisotropic nanochain array exhibits good biocompatibility and can guide the directional growth of nerve cells and the elongation of neurites. Upon in vivo application, the anisotropic nanochain array is transplanted into a 2-mm-long SCI area of rats and successfully promotes the regeneration of new neurons and axons, together with the recovery of motor functions. These findings suggest that magnetic nanochain-induced anisotropic nerve assembly can be a viable option for SCI repair.
{"title":"Magnetic nanochain-induced anisotropic nerve assembly for spinal cord injury repair","authors":"Yangnan Hu, Hao Wei, Hui Zhang, Hong Cheng, Dongyu Xu, Huan Wang, Zeyou Zhang, Bin Zhang, Yixian Liu, Yusong Wang, Chen Zhang, Jilai Li, Yuanjin Zhao, Renjie Chai","doi":"10.1016/j.cej.2024.157681","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157681","url":null,"abstract":"Utilizing neural tissue engineering scaffolds to improve and reconstruct the injury microenvironment has shown great promise for repairing spinal cord injury (SCI). Here, we present a type of magnetic nanochain-induced anisotropic nerve assembly for SCI repair. Under the magnetical drive, silica-coated magnetic nanoparticles assemble into highly stable nanochains, further integrated into the hydrogel and controlled by a magnetic field to form an anisotropic array in a three-dimensional space. In vitro studies confirm that the prepared anisotropic nanochain array exhibits good biocompatibility and can guide the directional growth of nerve cells and the elongation of neurites. Upon <em>in vivo</em> application, the anisotropic nanochain array is transplanted into a 2-mm-long SCI area of rats and successfully promotes the regeneration of new neurons and axons, together with the recovery of motor functions. These findings suggest that magnetic nanochain-induced anisotropic nerve assembly can be a viable option for SCI repair.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"98 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610286","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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