Pub Date : 2024-12-03DOI: 10.1016/j.chempr.2024.10.028
Boyang Zhang, Alexander B. Weberg, Andrew J. Ahn, Marta Guron, Leighton O. Jones, Michael R. Gau, George C. Schatz, Eric J. Schelter
Sustainable, cost-effective cobalt/nickel separations chemistry contributes to the realization of economically competitive lithium-ion battery recycling, as well as primary mining of cobalt and nickel. Such improvements can address supply chain challenges for cobalt, a critical element. Herein, we disclose a simple method for separating Co/Ni by second coordination-sphere molecular recognition. Selective cobalt precipitation is achieved using carbonate ions in an ammonia solution due to the outer-sphere, hydrogen bonding interactions between [Co(NH3)6]3+ and CO32−, evaluated with density functional theory calculations. We demonstrate this method on mixtures of Co/Ni chlorides comprising a 10-fold excess of Ni and provide comparisons with ore-processing systems. High purities (99.4(3)% Co; 98.2(4)% Ni) and recoveries (77(8)% Co; ∼100% Ni) were observed for both Co- and Ni-enriched products using optimized conditions. This method is potentially economically competitive based on initial techno-economic analysis (TEA) and life-cycle assessment (LCA) that also illustrate advantages in terms of sustainability.
{"title":"A sustainable cobalt separation with validation by techno-economic analysis and life-cycle assessment","authors":"Boyang Zhang, Alexander B. Weberg, Andrew J. Ahn, Marta Guron, Leighton O. Jones, Michael R. Gau, George C. Schatz, Eric J. Schelter","doi":"10.1016/j.chempr.2024.10.028","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.10.028","url":null,"abstract":"Sustainable, cost-effective cobalt/nickel separations chemistry contributes to the realization of economically competitive lithium-ion battery recycling, as well as primary mining of cobalt and nickel. Such improvements can address supply chain challenges for cobalt, a critical element. Herein, we disclose a simple method for separating Co/Ni by second coordination-sphere molecular recognition. Selective cobalt precipitation is achieved using carbonate ions in an ammonia solution due to the outer-sphere, hydrogen bonding interactions between [Co(NH<sub>3</sub>)<sub>6</sub>]<sup>3+</sup> and CO<sub>3</sub><sup>2−</sup>, evaluated with density functional theory calculations. We demonstrate this method on mixtures of Co/Ni chlorides comprising a 10-fold excess of Ni and provide comparisons with ore-processing systems. High purities (99.4(3)% Co; 98.2(4)% Ni) and recoveries (77(8)% Co; ∼100% Ni) were observed for both Co- and Ni-enriched products using optimized conditions. This method is potentially economically competitive based on initial techno-economic analysis (TEA) and life-cycle assessment (LCA) that also illustrate advantages in terms of sustainability.","PeriodicalId":268,"journal":{"name":"Chem","volume":"9 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142760253","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-12-03DOI: 10.1016/j.chempr.2024.10.024
Ruozhou Huang, Yuping Wang
In a recent issue of Chem, an innovative approach for the synthesis of crystalline [2]catenane-containing covalent organic frameworks was developed. This breakthrough elucidates how the dynamics of microscopic, interlocked components influence material properties, thereby advancing the design of two-dimensional materials with sophisticated topological features.
{"title":"Ordered [2]catenanes in covalent organic frameworks: From molecules to materials","authors":"Ruozhou Huang, Yuping Wang","doi":"10.1016/j.chempr.2024.10.024","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.10.024","url":null,"abstract":"In a recent issue of <em>Chem</em>, an innovative approach for the synthesis of crystalline [2]catenane-containing covalent organic frameworks was developed. This breakthrough elucidates how the dynamics of microscopic, interlocked components influence material properties, thereby advancing the design of two-dimensional materials with sophisticated topological features.","PeriodicalId":268,"journal":{"name":"Chem","volume":"116 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142760252","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-12-02DOI: 10.1016/j.chempr.2024.10.029
Huai Qin Fu, Tingting Yu, Jessica White, Ji Wei Sun, Yuming Wu, Wen Jing Li, Nicholas M. Bedford, Yun Wang, Thomas E. Rufford, Cheng Lian, Porun Liu, Hua Gui Yang, Huijun Zhao
The path to practical production of targeted chemicals and fuels application via carbon dioxide reduction reactions (CO2RRs) remains a significant challenge mainly due to low CO2 solubility. Aiming to tackle this key issue, herein, we used the CuSbOx cathode-catalyzed reduction of CO2 to CO as a model system to quantitatively depict CO2 demand-supply and performance relationships. We propose a cathode/electrolyte interface model consisting of a porous catalyst layer, and we combined the experimental and computational COMSOL Multiphysics finite-element studies to quantitatively unveil CO2 demand-supply relationships and determine the maximum CO2 supply capacity in both stationary H cell and gas diffusion electrode (GDE) flow cell. This work exemplifies that experimentally measured catalytic performance may not accurately reflect the maximum capacity/intrinsic electrocatalytic activity of electrocatalysts and reveals that CO2 supply capacity in the GDE flow cell can be dramatically affected by the thickness of the liquid layer between the hydrophobic gas diffusion layer and the catalyst layer.
{"title":"Amorphous CuSbOx composite-catalyzed electrocatalytic reduction of CO2 to CO: CO2 demand-supply-regulated performance","authors":"Huai Qin Fu, Tingting Yu, Jessica White, Ji Wei Sun, Yuming Wu, Wen Jing Li, Nicholas M. Bedford, Yun Wang, Thomas E. Rufford, Cheng Lian, Porun Liu, Hua Gui Yang, Huijun Zhao","doi":"10.1016/j.chempr.2024.10.029","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.10.029","url":null,"abstract":"The path to practical production of targeted chemicals and fuels application via carbon dioxide reduction reactions (CO<sub>2</sub>RRs) remains a significant challenge mainly due to low CO<sub>2</sub> solubility. Aiming to tackle this key issue, herein, we used the CuSbO<sub>x</sub> cathode-catalyzed reduction of CO<sub>2</sub> to CO as a model system to quantitatively depict CO<sub>2</sub> demand-supply and performance relationships. We propose a cathode/electrolyte interface model consisting of a porous catalyst layer, and we combined the experimental and computational COMSOL Multiphysics finite-element studies to quantitatively unveil CO<sub>2</sub> demand-supply relationships and determine the maximum CO<sub>2</sub> supply capacity in both stationary H cell and gas diffusion electrode (GDE) flow cell. This work exemplifies that experimentally measured catalytic performance may not accurately reflect the maximum capacity/intrinsic electrocatalytic activity of electrocatalysts and reveals that CO<sub>2</sub> supply capacity in the GDE flow cell can be dramatically affected by the thickness of the liquid layer between the hydrophobic gas diffusion layer and the catalyst layer.","PeriodicalId":268,"journal":{"name":"Chem","volume":"3 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758663","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-29DOI: 10.1016/j.chempr.2024.10.025
Amol Uttam Pawar, Ramesh Poonchi Sivasankaran, Long Yang, Don Keun Lee, Young Soo Kang
Solar-to-fuel production via the carbon dioxide (CO2) reduction reaction (CO2RR) is a crucial and widely discussed topic, particularly in the context of climate change. Electro-solar approaches, such as electrochemical (EC), photochemical (PC), and photoelectrochemical (PEC) methods, are promising for CO2RR due to their efficiency and mild operating conditions. The process of converting CO2 into valuable products involves multiple steps and requires a deep understanding of reaction mechanisms and product selectivity. In situ and operando spectroscopic techniques are essential for elucidating these mechanisms. This review focuses on advanced in situ spectroscopic methods, such as X-ray absorption spectroscopy (XAS), infrared (IR) spectroscopy, Raman spectroscopy, and electron paramagnetic resonance (EPR) spectroscopy, which provide insights into CO2 adsorption, activation, and electron-proton transfer, leading to intermediate radical formation. Additionally, advanced X-ray techniques are briefly discussed, offering refined approaches to studying CO2RR dynamics. These integrated techniques are crucial for designing and optimizing catalysts for efficient CO2 reduction and conversion.
{"title":"A methodical strategy for achieving efficient electro-solar reduction, incorporating appropriate in situ techniques","authors":"Amol Uttam Pawar, Ramesh Poonchi Sivasankaran, Long Yang, Don Keun Lee, Young Soo Kang","doi":"10.1016/j.chempr.2024.10.025","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.10.025","url":null,"abstract":"Solar-to-fuel production via the carbon dioxide (CO<sub>2</sub>) reduction reaction (CO2RR) is a crucial and widely discussed topic, particularly in the context of climate change. Electro-solar approaches, such as electrochemical (EC), photochemical (PC), and photoelectrochemical (PEC) methods, are promising for CO2RR due to their efficiency and mild operating conditions. The process of converting CO<sub>2</sub> into valuable products involves multiple steps and requires a deep understanding of reaction mechanisms and product selectivity. <em>In situ</em> and <em>operando</em> spectroscopic techniques are essential for elucidating these mechanisms. This review focuses on advanced <em>in situ</em> spectroscopic methods, such as X-ray absorption spectroscopy (XAS), infrared (IR) spectroscopy, Raman spectroscopy, and electron paramagnetic resonance (EPR) spectroscopy, which provide insights into CO<sub>2</sub> adsorption, activation, and electron-proton transfer, leading to intermediate radical formation. Additionally, advanced X-ray techniques are briefly discussed, offering refined approaches to studying CO2RR dynamics. These integrated techniques are crucial for designing and optimizing catalysts for efficient CO<sub>2</sub> reduction and conversion.","PeriodicalId":268,"journal":{"name":"Chem","volume":"259 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142742537","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-26DOI: 10.1016/j.chempr.2024.09.032
James M. Gallagher, Joaquin Baixeras Buye, David A. Leigh
Biological cells sustain an out-of-equilibrium state by harnessing energy flows across compartment boundaries. In this issue of Chem, Penocchio et al. quantify how out-of-equilibrium chemical reaction networks respond to compartmentalization—providing a framework on which to build and understand aspects of nonequilibrium self-assembly, molecular machinery, and other endergonic processes.
{"title":"Out-of-equilibrium compartments: Thinking inside the box","authors":"James M. Gallagher, Joaquin Baixeras Buye, David A. Leigh","doi":"10.1016/j.chempr.2024.09.032","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.09.032","url":null,"abstract":"Biological cells sustain an out-of-equilibrium state by harnessing energy flows across compartment boundaries. In this issue of <em>Chem</em>, Penocchio et al. quantify how out-of-equilibrium chemical reaction networks respond to compartmentalization—providing a framework on which to build and understand aspects of nonequilibrium self-assembly, molecular machinery, and other endergonic processes.","PeriodicalId":268,"journal":{"name":"Chem","volume":"4 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142719061","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-22DOI: 10.1016/j.chempr.2024.11.001
Jessica Liane Hübner, Gina Ruland, Florian Pietschmann, Zita Brejwo, Benjamin Paul, Peter Strasser
The electrolyte design plays a key, yet underexplored, role in the two-electron oxygen reduction reaction (2e− ORR) to hydrogen peroxide (H2O2). Here, we investigate the dramatic beneficial impact of alkali metal cations (AMCs) on the H2O2 production in commercial carbon gas diffusion electrode-based flow electrolyzers in single-pass and closed-loop modes using online analytics. We demonstrate previously unavailable single-pass H2O2 production rates of up to 123 mg cm−2 h−1 with a Faraday efficiency (FE) of 96.9% at −200 mA cm−2 in the presence of potassium cations, exceeding the corresponding production rate and FE in 0.1 M H2SO4 by a factor of 34. Additionally, to the increased selectivity, the onset potential of the 2e− ORR shifted by 0.42 V toward a less negative potential. Furthermore, we explore and quantify the influence of multivalent metal cations (Ca2+, Mg2+, and Al3+) on the 2e− ORR.
{"title":"Electrolyte design for high hydrogen peroxide production rates utilizing commercial carbon gas diffusion electrodes","authors":"Jessica Liane Hübner, Gina Ruland, Florian Pietschmann, Zita Brejwo, Benjamin Paul, Peter Strasser","doi":"10.1016/j.chempr.2024.11.001","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.11.001","url":null,"abstract":"The electrolyte design plays a key, yet underexplored, role in the two-electron oxygen reduction reaction (2e<sup>−</sup> ORR) to hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>). Here, we investigate the dramatic beneficial impact of alkali metal cations (AMCs) on the H<sub>2</sub>O<sub>2</sub> production in commercial carbon gas diffusion electrode-based flow electrolyzers in single-pass and closed-loop modes using online analytics. We demonstrate previously unavailable single-pass H<sub>2</sub>O<sub>2</sub> production rates of up to 123 mg cm<sup>−2</sup> h<sup>−1</sup> with a Faraday efficiency (FE) of 96.9% at −200 mA cm<sup>−2</sup> in the presence of potassium cations, exceeding the corresponding production rate and FE in 0.1 M H<sub>2</sub>SO<sub>4</sub> by a factor of 34. Additionally, to the increased selectivity, the onset potential of the 2e<sup>−</sup> ORR shifted by 0.42 V toward a less negative potential. Furthermore, we explore and quantify the influence of multivalent metal cations (Ca<sup>2+</sup>, Mg<sup>2+</sup>, and Al<sup>3+</sup>) on the 2e<sup>−</sup> ORR.","PeriodicalId":268,"journal":{"name":"Chem","volume":"4 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142684995","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-22DOI: 10.1016/j.chempr.2024.10.009
Javier Corpas, Eva Rivera-Chao, Enrique M. Arpa, Miguel Gomez-Mendoza, Yuri Katayama, Victor A. de la Peña O’Shea, Céline Bouchel, Clément Jacob, Pierre-Georges Echeverria, Alessandro Ruffoni, Daniele Leonori
The Birch reaction is a classical process used for the partial reduction of aromatics into non-conjugated cyclohexadienes that can be further functionalized. This strategy and its more modern variants are all based on an initial single-electron transfer event converting the arene into the corresponding radical anion for either protonation or hydrogen-atom transfer. Herein, we demonstrate an umpolung approach where the aromatic is first protonated to its corresponding carbocation and then reduced using the Lewis acid-base complex Et3N−BH3. This strategy requires aromatic photoexcitation so that protonation is favored by charge-transfer and driven by excited-state antiaromaticity relief. This means that aromatic excited-state basicity rather than ground-state redox potential needs to be considered when approaching reaction development. The mild conditions and the avoidance of strong reductants have enabled tolerance of functionalities generally not compatible under standard Birch conditions.
{"title":"Excited-state protonation and reduction enables the umpolung Birch reduction of naphthalenes","authors":"Javier Corpas, Eva Rivera-Chao, Enrique M. Arpa, Miguel Gomez-Mendoza, Yuri Katayama, Victor A. de la Peña O’Shea, Céline Bouchel, Clément Jacob, Pierre-Georges Echeverria, Alessandro Ruffoni, Daniele Leonori","doi":"10.1016/j.chempr.2024.10.009","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.10.009","url":null,"abstract":"The Birch reaction is a classical process used for the partial reduction of aromatics into non-conjugated cyclohexadienes that can be further functionalized. This strategy and its more modern variants are all based on an initial single-electron transfer event converting the arene into the corresponding radical anion for either protonation or hydrogen-atom transfer. Herein, we demonstrate an umpolung approach where the aromatic is first protonated to its corresponding carbocation and then reduced using the Lewis acid-base complex Et<sub>3</sub>N−BH<sub>3</sub>. This strategy requires aromatic photoexcitation so that protonation is favored by charge-transfer and driven by excited-state antiaromaticity relief. This means that aromatic excited-state basicity rather than ground-state redox potential needs to be considered when approaching reaction development. The mild conditions and the avoidance of strong reductants have enabled tolerance of functionalities generally not compatible under standard Birch conditions.","PeriodicalId":268,"journal":{"name":"Chem","volume":"37 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142684996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Preparation for the potential emergence of future human coronaviruses (HCoVs) calls for the development of versatile and effective treatment strategies. The signs and symptoms of HCoVs include an immune inflammatory response. Therefore, our study focuses on the simultaneous inhibition of HCoV infection and the alleviation of lung inflammation. Inspired by conformational epitope matching, we engineered a de novo antigen spatial-matching polyaptamer (ASM-pApt) nanostructure designed to align perfectly with multiple spike (S) proteins on severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) pseudovirus (PsV). Compared with monovalent aptamer, the dissociation constant (KD) of the ASM-pApt nanostructure decreased by over 1,000-fold, and its viral semi-inhibitory concentration (IC50) improved by over 100,000-fold to 89.7 fM (fmol/L), indicating the effectiveness of antigen spatial matching. By loading polyphenol as anti-inflammatory drug and chitosan (CS) as an excipient, the ASM-pApt nanostructure showed anti-inflammatory and long drug retention properties. Our design shows the promise of polyaptamer as an antiviral/anti-inflammatory candidate against emerging HCoVs in the future.
{"title":"Antigen spatial-matching polyaptamer nanostructure to block coronavirus infection and alleviate inflammation","authors":"Jingqi Chen, Yuqing Li, Xueliang Liu, Hongyi Li, Jiawei Zhu, Rui Ma, Linxin Tian, Lu Yu, Jiabei Li, Zhuang Liu, Weihong Tan, Yu Yang","doi":"10.1016/j.chempr.2024.10.021","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.10.021","url":null,"abstract":"Preparation for the potential emergence of future human coronaviruses (HCoVs) calls for the development of versatile and effective treatment strategies. The signs and symptoms of HCoVs include an immune inflammatory response. Therefore, our study focuses on the simultaneous inhibition of HCoV infection and the alleviation of lung inflammation. Inspired by conformational epitope matching, we engineered a <em>de novo</em> antigen spatial-matching polyaptamer (ASM-pApt) nanostructure designed to align perfectly with multiple spike (S) proteins on severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) pseudovirus (PsV). Compared with monovalent aptamer, the dissociation constant (K<sub>D</sub>) of the ASM-pApt nanostructure decreased by over 1,000-fold, and its viral semi-inhibitory concentration (IC<sub>50</sub>) improved by over 100,000-fold to 89.7 fM (fmol/L), indicating the effectiveness of antigen spatial matching. By loading polyphenol as anti-inflammatory drug and chitosan (CS) as an excipient, the ASM-pApt nanostructure showed anti-inflammatory and long drug retention properties. Our design shows the promise of polyaptamer as an antiviral/anti-inflammatory candidate against emerging HCoVs in the future.","PeriodicalId":268,"journal":{"name":"Chem","volume":"2 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678776","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-21DOI: 10.1016/j.chempr.2024.10.023
Gabriel Sanchez-Cano, Pablo Cristobal-Cueto, Lydia Saez, Antonio Lastra, Ana Marti-Calvo, Juan José Gutiérrez-Sevillano, Sofía Calero, Sara Rojas, Patricia Horcajada
Water disinfection is one of the most challenging processes for public health. Nevertheless, this process can generate inorganic by-products (chlorite [ClO2−] and chlorate [ClO3−]) associated with human diseases. Recently, the European Union established a permissible maximum concentration of 0.25 mg⋅L−1 for both oxyanions in drinking water; thus, the existing technologies have to be adapted. Here, the earliest use of metal-organic frameworks (MOFs) in the elimination of the disinfection by-products ClO2− and ClO3− from fresh water is presented. Among the Fe-MOFs proposed, the robust MIL-88B-NH2 demonstrated exceptional oxyanions elimination capacities (100% and 30% of ClO2− and ClO3− in 1 and 5 min, respectively). Based on these results, a continuous-flow device based on MIL-88B-NH2 was tested under simulated realistic conditions, achieving high oxyanions elimination capacities, and the reusability of the system was demonstrated. This pioneering work opens new perspectives in the implementation of MOFs in real drinking water treatment plants (DWTPs).
{"title":"Drinking water purification using metal-organic frameworks: Removal of disinfection by-products","authors":"Gabriel Sanchez-Cano, Pablo Cristobal-Cueto, Lydia Saez, Antonio Lastra, Ana Marti-Calvo, Juan José Gutiérrez-Sevillano, Sofía Calero, Sara Rojas, Patricia Horcajada","doi":"10.1016/j.chempr.2024.10.023","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.10.023","url":null,"abstract":"Water disinfection is one of the most challenging processes for public health. Nevertheless, this process can generate inorganic by-products (chlorite [ClO<sub>2</sub><sup>−</sup>] and chlorate [ClO<sub>3</sub><sup>−</sup>]) associated with human diseases. Recently, the European Union established a permissible maximum concentration of 0.25 mg⋅L<sup>−1</sup> for both oxyanions in drinking water; thus, the existing technologies have to be adapted. Here, the earliest use of metal-organic frameworks (MOFs) in the elimination of the disinfection by-products ClO<sub>2</sub><sup>−</sup> and ClO<sub>3</sub><sup>−</sup> from fresh water is presented. Among the Fe-MOFs proposed, the robust MIL-88B-NH<sub>2</sub> demonstrated exceptional oxyanions elimination capacities (100% and 30% of ClO<sub>2</sub><sup>−</sup> and ClO<sub>3</sub><sup>−</sup> in 1 and 5 min, respectively). Based on these results, a continuous-flow device based on MIL-88B-NH<sub>2</sub> was tested under simulated realistic conditions, achieving high oxyanions elimination capacities, and the reusability of the system was demonstrated. This pioneering work opens new perspectives in the implementation of MOFs in real drinking water treatment plants (DWTPs).","PeriodicalId":268,"journal":{"name":"Chem","volume":"14 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678749","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-20DOI: 10.1016/j.chempr.2024.10.018
Wentao Song, Xinyue Zhang, Wanrong Li, Bowen Li, Bin Liu
Constructing biotic-abiotic hybrid systems for solar energy conversion receives growing interest owing to their sustainable and eco-friendly approach to producing chemicals. The integration of intracellular biochemical pathways with semiconductor materials offers superior product selectivity and efficient light utilization in solar-driven biocatalysis. However, the complicated multidisciplinary features and limited understanding of extracellular electron transfer at the biological-material interfaces hinder the practical application of biotic-abiotic hybrid systems for converting solar energy. In this perspective, we summarize the fundamental mechanisms of biohybrid systems for solar-to-chemical conversion and highlight ongoing challenges and promising directions for future development. First, a comprehensive overview of biotic-abiotic hybrid systems is introduced together with the mechanism of extracellular electron transfer for chemical production. Then, recent achievements of biohybrid systems for H2 production, CO2 reduction, N2 fixation, and chemical synthesis are discussed in detail. Finally, the current challenges in biotic-abiotic hybrid systems and prospective research directions are explored.
{"title":"Engineering biotic-abiotic hybrid systems for solar-to-chemical conversion","authors":"Wentao Song, Xinyue Zhang, Wanrong Li, Bowen Li, Bin Liu","doi":"10.1016/j.chempr.2024.10.018","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.10.018","url":null,"abstract":"Constructing biotic-abiotic hybrid systems for solar energy conversion receives growing interest owing to their sustainable and eco-friendly approach to producing chemicals. The integration of intracellular biochemical pathways with semiconductor materials offers superior product selectivity and efficient light utilization in solar-driven biocatalysis. However, the complicated multidisciplinary features and limited understanding of extracellular electron transfer at the biological-material interfaces hinder the practical application of biotic-abiotic hybrid systems for converting solar energy. In this perspective, we summarize the fundamental mechanisms of biohybrid systems for solar-to-chemical conversion and highlight ongoing challenges and promising directions for future development. First, a comprehensive overview of biotic-abiotic hybrid systems is introduced together with the mechanism of extracellular electron transfer for chemical production. Then, recent achievements of biohybrid systems for H<sub>2</sub> production, CO<sub>2</sub> reduction, N<sub>2</sub> fixation, and chemical synthesis are discussed in detail. Finally, the current challenges in biotic-abiotic hybrid systems and prospective research directions are explored.","PeriodicalId":268,"journal":{"name":"Chem","volume":"23 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673764","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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