ACS Central Science最新文献_第3页

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-11-06 eCollection Date: 2024-11-27 DOI: 10.1021/acscentsci.4c01803

Ute Eberle

引用次数: 0

Overcoming the Limitations of Transition-Metal Catalysis in the Chemoenzymatic Dynamic Kinetic Resolution (DKR) of Atropisomeric Bisnaphthols 克服过渡金属催化在异构双萘酚化学动态动力学解析 (DKR) 中的局限性

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-11-05 DOI: 10.1021/acscentsci.4c0137010.1021/acscentsci.4c01370

Kun Wang, Wei Wang, Dingkai Lou, Jie Zhang, Changli Chi, Jan-E. Bäckvall*, Xiang Sheng* and Can Zhu*,

{"title":"Overcoming the Limitations of Transition-Metal Catalysis in the Chemoenzymatic Dynamic Kinetic Resolution (DKR) of Atropisomeric Bisnaphthols","authors":"Kun Wang, Wei Wang, Dingkai Lou, Jie Zhang, Changli Chi, Jan-E. Bäckvall*, Xiang Sheng* and Can Zhu*, ","doi":"10.1021/acscentsci.4c0137010.1021/acscentsci.4c01370","DOIUrl":"https://doi.org/10.1021/acscentsci.4c01370https://doi.org/10.1021/acscentsci.4c01370","url":null,"abstract":"Chemoenzymatic dynamic kinetic resolution (DKR), combining a metal racemization catalyst with an enzyme, has emerged as an elegant solution to transform racemic substrates into enantiopure products, while compatibility of dual catalysis is the key issue. Conventional solutions have utilized presynthesized metal complexes with a fixed and bulky ligand to protect the metal from the enzyme system; however, this has been generally limited to anionic ligands. Herein, we report our strategy to solve the compatibility issue by employing a reliable ligand that firmly coordinates in situ to the metal. Such a reliable ligand offers π* orbitals, allowing additional metal-to-ligand d−π* back-donation, which can significantly enhance coordination effects between the ligand and metal. Therefore, we developed an efficient DKR method to access chiral BINOLs from racemic derivatives under dual copper and enzyme catalysis. In cooperation with lipase LPL-311-Celite, the DKR of BINOLs was successfully realized with a copper catalyst via in situ coordination of BCP (L8) to CuCl. A series of functionalized C2- and C1-symmetric chiral biaryls could be synthesized in high yields with good enantioselectivity. The racemization mechanism was proposed to involve a radical-anion intermediate, which allows the axial rotation with a dramatic decrease of the rotation barrier.A bathocuproine ligand offers d−π* back-donation to enhance the coordination effect in copper catalysis to enable the chemoenzymatic dynamic kinetic resolution (DKR) of atropisomeric bisnaphthols.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"10 11","pages":"2099–2110 2099–2110"},"PeriodicalIF":12.7,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c01370","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142719104","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Overcoming the Limitations of Transition-Metal Catalysis in the Chemoenzymatic Dynamic Kinetic Resolution (DKR) of Atropisomeric Bisnaphthols.

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-11-05 eCollection Date: 2024-11-27 DOI: 10.1021/acscentsci.4c01370

Kun Wang, Wei Wang, Dingkai Lou, Jie Zhang, Changli Chi, Jan-E Bäckvall, Xiang Sheng, Can Zhu

{"title":"Overcoming the Limitations of Transition-Metal Catalysis in the Chemoenzymatic Dynamic Kinetic Resolution (DKR) of Atropisomeric Bisnaphthols.","authors":"Kun Wang, Wei Wang, Dingkai Lou, Jie Zhang, Changli Chi, Jan-E Bäckvall, Xiang Sheng, Can Zhu","doi":"10.1021/acscentsci.4c01370","DOIUrl":"10.1021/acscentsci.4c01370","url":null,"abstract":"Chemoenzymatic dynamic kinetic resolution (DKR), combining a metal racemization catalyst with an enzyme, has emerged as an elegant solution to transform racemic substrates into enantiopure products, while compatibility of dual catalysis is the key issue. Conventional solutions have utilized presynthesized metal complexes with a fixed and bulky ligand to protect the metal from the enzyme system; however, this has been generally limited to anionic ligands. Herein, we report our strategy to solve the compatibility issue by employing a reliable ligand that firmly coordinates in situ to the metal. Such a reliable ligand offers π* orbitals, allowing additional metal-to-ligand d-π* back-donation, which can significantly enhance coordination effects between the ligand and metal. Therefore, we developed an efficient DKR method to access chiral BINOLs from racemic derivatives under dual copper and enzyme catalysis. In cooperation with lipase LPL-311-Celite, the DKR of BINOLs was successfully realized with a copper catalyst via in situ coordination of BCP (L8) to CuCl. A series of functionalized C 2- and C 1-symmetric chiral biaryls could be synthesized in high yields with good enantioselectivity. The racemization mechanism was proposed to involve a radical-anion intermediate, which allows the axial rotation with a dramatic decrease of the rotation barrier.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"10 11","pages":"2099-2110"},"PeriodicalIF":12.7,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11613327/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142778826","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Highly Efficient Degradation of Emerging Contaminants with Sodium Bicarbonate-Enhanced Mn(II)/Peracetic Acid Process: Formation and Contribution of Mn(V) 利用碳酸氢钠增强型锰（II）/过乙酸工艺高效降解新污染物：锰（V）的形成和贡献

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-11-03 DOI: 10.1021/acs.est.4c0687810.1021/acs.est.4c06878

Linfeng He, Jing Zou*, Jianying Wu, Sheng Li, Zhijie Wu, Yixin Huang, Xiaoya Kou, Qingfeng Cheng, Panpan Wang and Jun Ma,

{"title":"Highly Efficient Degradation of Emerging Contaminants with Sodium Bicarbonate-Enhanced Mn(II)/Peracetic Acid Process: Formation and Contribution of Mn(V)","authors":"Linfeng He, Jing Zou*, Jianying Wu, Sheng Li, Zhijie Wu, Yixin Huang, Xiaoya Kou, Qingfeng Cheng, Panpan Wang and Jun Ma, ","doi":"10.1021/acs.est.4c0687810.1021/acs.est.4c06878","DOIUrl":"https://doi.org/10.1021/acs.est.4c06878https://doi.org/10.1021/acs.est.4c06878","url":null,"abstract":"Organic ligands have been extensively used to enhance the catalytic performance of manganese ion (Mn(II)) for peracetic acid (PAA). In this study, sodium bicarbonate (NaHCO3), an economical and eco-friendly inorganic ligand, was introduced to enhance the degradation of emerging contaminants (ECs) in the Mn(II)/PAA process. NaHCO3 could significantly improve the oxidizing ability of the Mn(II)/PAA process over the initial pH range of 3.0–11.0. Mn(V) was identified as the primary reactive species for degrading naproxen in the NaHCO3/Mn(II)/PAA process. HCO3– could complex with Mn(II) to generate Mn(II)-HCO3–, which has a lower redox potential to enhance the catalytic activity of Mn(II). Mn(II)-HCO3– reacted with PAA to produce Mn(III)-HCO3– and CH3C(O)O•. Mn(V)-HCO3– was generated via two-electron transfer between Mn(III)-HCO3– and PAA. Although organic radicals were detected in the NaHCO3/Mn(II)/PAA process, naproxen was mainly degraded by Mn(V)-HCO3– via one-electron transfer along with the formation of MnO2. Notably, the coexisting hydrogen peroxide was vital in the reduction of MnO2 to Mn(II/III), thereby enhancing the continuous generation of Mn(V)-HCO3–. NaHCO3/Mn(II)/PAA process exhibited exceptional oxidation performance in actual water samples. This study proposed a strategy utilizing an eco-friendly inorganic ligand to address the inherent drawbacks of organic ligand-enhanced Mn(II)/PAA processes and highlighted its potential applications in the removal of ECs.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20313–20326 20313–20326"},"PeriodicalIF":10.8,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608529","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}

引用次数: 0

Geochemical Decoupling of Iron and Zinc during Transformation of Zn-Bearing Ferrihydrite in Reducing Sediments 还原沉积物中含锌铁酸盐转化过程中铁和锌的地球化学脱钩

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-11-03 DOI: 10.1021/acs.est.4c0926110.1021/acs.est.4c09261

Pierre Lefebvre*, Andrew R. C. Grigg and Ruben Kretzschmar,

{"title":"Geochemical Decoupling of Iron and Zinc during Transformation of Zn-Bearing Ferrihydrite in Reducing Sediments","authors":"Pierre Lefebvre*, Andrew R. C. Grigg and Ruben Kretzschmar, ","doi":"10.1021/acs.est.4c0926110.1021/acs.est.4c09261","DOIUrl":"https://doi.org/10.1021/acs.est.4c09261https://doi.org/10.1021/acs.est.4c09261","url":null,"abstract":"The transformation of the mineral ferrihydrite in reducing environments, and its impact on the mobility of incorporated trace metals, has been investigated in model laboratory studies, but studies using complex soil or sediment matrices are lacking. Here, we studied the transformation of zinc (Zn)-bearing ferrihydrite labeled with 57Fe and mixed with natural sediments, incubated in reducing conditions for up to six months. We tracked the evolution of Fe and Zn speciation with 57Fe Mössbauer spectroscopy and with bulk and micro-X-ray absorption spectroscopy. We show that Fe was readily reduced and incorporated into a poorly crystalline mixed-valence Fe(II)–Fe(III) phase resembling green rust. In parallel, Zn was released in the surrounding porewater and scavenged by precipitation with available ligands, particularly as zinc sulfide (ZnS) or Zn-carbonates. Early in the mineral transformation process, the chemical behavior of Fe was decoupled from Zn, suppressing the impact of Zn on the rates and products of the ferrihydrite transformation. Our results underline the discrepancy between model experiments and complex field-like conditions and highlight the importance of sediment and soil geochemistry and ligand competition on the fate of divalent metal contaminants in the environment.We investigated the in situ mineral transformation of Zn-bearing ferrihydrite in natural sediments, showing that Zn and Fe behave differently and incorporate into different mineral products, in contrast with model laboratory studies.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20224–20234 20224–20234"},"PeriodicalIF":10.8,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.est.4c09261","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608530","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

An Ambient Measurement Technique for Vehicle Emission Quantification and Concentration Source Apportionment 用于车辆排放定量和浓度源分配的环境测量技术

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-11-03 DOI: 10.1021/acs.est.4c0790710.1021/acs.est.4c07907

Naomi J. Farren, Samuel Wilson, Yoann Bernard, Marvin D. Shaw, Kaylin Lee, Mallery Crowe and David C. Carslaw*,

{"title":"An Ambient Measurement Technique for Vehicle Emission Quantification and Concentration Source Apportionment","authors":"Naomi J. Farren, Samuel Wilson, Yoann Bernard, Marvin D. Shaw, Kaylin Lee, Mallery Crowe and David C. Carslaw*, ","doi":"10.1021/acs.est.4c0790710.1021/acs.est.4c07907","DOIUrl":"https://doi.org/10.1021/acs.est.4c07907https://doi.org/10.1021/acs.est.4c07907","url":null,"abstract":"We develop a new technique called plume regression where fast response instruments located at the roadside are used to measure exhaust plumes of passing vehicles. The approach is used to generate highly disaggregated vehicle emissions information by vehicle type, which compares well with traditional vehicle emission remote sensing. Additionally, the technique provides valuable new information on ambient concentration source apportionment by vehicle type. The technique is flexible enough to consider a wide range of air pollutants and be deployed at roadside ambient monitoring locations. The new approach is used to quantify emissions and concentration source apportionment for ammonia (NH3) and nitrogen oxides (NOx). We find that emissions of NH3 are generally very well controlled from diesel vehicles including those with selective catalytic reduction systems that use NH3 to reduce emissions of NOx. By contrast, gasoline passenger cars are shown to be the dominant contributor to NH3 emissions, which increase with vehicle mileage. Average fuel-specific NH3 emission factors for gasoline vehicles range from 0.3 to 1.2 g kg–1, while diesel vehicle emission factors remain below 0.06 g kg–1, with the exception of Euro VI buses with the latest regulatory provisions (0.5 g kg–1).Emission control technologies have led to reduced but increasingly complex emissions from the transport sector. We present a new technique to characterize these emissions and apportion roadside pollutant concentrations to specific vehicle types.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20091–20100 20091–20100"},"PeriodicalIF":10.8,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.est.4c07907","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608534","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

High-Affinity Peptides for Target Protein Screened in Ultralarge Virtual Libraries 在超大虚拟文库中筛选目标蛋白的高亲和性多肽

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-11-02 DOI: 10.1021/acscentsci.4c0138510.1021/acscentsci.4c01385

Boyuan Xue, Ruixue Li, Zhao Cheng and Xiaohong Zhou*,

{"title":"High-Affinity Peptides for Target Protein Screened in Ultralarge Virtual Libraries","authors":"Boyuan Xue, Ruixue Li, Zhao Cheng and Xiaohong Zhou*, ","doi":"10.1021/acscentsci.4c0138510.1021/acscentsci.4c01385","DOIUrl":"https://doi.org/10.1021/acscentsci.4c01385https://doi.org/10.1021/acscentsci.4c01385","url":null,"abstract":"High-throughput virtual screening (HTVS) has emerged as a pivotal strategy for identifying high-affinity peptides targeting functional proteins, which are crucial for diagnostic and therapeutic applications. In the HTVS of peptides, expanding the library capacity to enhance peptide sequence diversity, thereby screening out excellent affinity peptide candidates, remains a significant challenge. This study presents a de novo design strategy that leverages directed mutation driven HTVS to evolve vast virtual libraries and screen peptides with ultrahigh affinities for various target proteins. Utilizing a computer-generated library of 104 random 15-mer peptide scaffolds, we employed a self-developed algorithm for parallelized HTVS with Autodock Vina. The top 1% of designs underwent random mutations at a rate of 20% for six generations, theoretically expanding the library to 1014 members. This approach was applied to various protein targets, including a tumor marker (alpha fetoprotein, AFP) and virus surface proteins (SARS-CoV-2 RBD and norovirus P-domain). Starting from the same 104 random 15-mer peptide library, peptides with high affinities in the nanomolar range for three protein targets were successfully identified. The energy-saving and high-efficient design strategy presents new opportunities for the cost-effective development of more effective high-affinity peptides for various environmental and health applications.This work devised a de novo design strategy that leverages directed mutation driven HTVS to evolve vast virtual libraries and screen peptides with ultrahigh affinities for various target proteins.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"10 11","pages":"2111–2118 2111–2118"},"PeriodicalIF":12.7,"publicationDate":"2024-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c01385","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142719497","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

High-Affinity Peptides for Target Protein Screened in Ultralarge Virtual Libraries.

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-11-02 eCollection Date: 2024-11-27 DOI: 10.1021/acscentsci.4c01385

Boyuan Xue, Ruixue Li, Zhao Cheng, Xiaohong Zhou

{"title":"High-Affinity Peptides for Target Protein Screened in Ultralarge Virtual Libraries.","authors":"Boyuan Xue, Ruixue Li, Zhao Cheng, Xiaohong Zhou","doi":"10.1021/acscentsci.4c01385","DOIUrl":"10.1021/acscentsci.4c01385","url":null,"abstract":"High-throughput virtual screening (HTVS) has emerged as a pivotal strategy for identifying high-affinity peptides targeting functional proteins, which are crucial for diagnostic and therapeutic applications. In the HTVS of peptides, expanding the library capacity to enhance peptide sequence diversity, thereby screening out excellent affinity peptide candidates, remains a significant challenge. This study presents a de novo design strategy that leverages directed mutation driven HTVS to evolve vast virtual libraries and screen peptides with ultrahigh affinities for various target proteins. Utilizing a computer-generated library of 104 random 15-mer peptide scaffolds, we employed a self-developed algorithm for parallelized HTVS with Autodock Vina. The top 1% of designs underwent random mutations at a rate of 20% for six generations, theoretically expanding the library to 1014 members. This approach was applied to various protein targets, including a tumor marker (alpha fetoprotein, AFP) and virus surface proteins (SARS-CoV-2 RBD and norovirus P-domain). Starting from the same 104 random 15-mer peptide library, peptides with high affinities in the nanomolar range for three protein targets were successfully identified. The energy-saving and high-efficient design strategy presents new opportunities for the cost-effective development of more effective high-affinity peptides for various environmental and health applications.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"10 11","pages":"2111-2118"},"PeriodicalIF":12.7,"publicationDate":"2024-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11613273/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142778747","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Predicting Behavior and Fate of Atmospheric Mercury in Soils: Age-Dating METAALICUS Hg Isotope Spikes with Fallout Radionuclide Chronometry 预测大气中的汞在土壤中的行为和归宿：利用落尘放射性核素年代测定法确定 METAALICUS 汞同位素尖峰的年代

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-11-02 DOI: 10.1021/acs.est.4c0154410.1021/acs.est.4c01544

Joshua D. Landis*, Vivien F. Taylor, Holger Hintelmann and Lee E. Hrenchuk,

{"title":"Predicting Behavior and Fate of Atmospheric Mercury in Soils: Age-Dating METAALICUS Hg Isotope Spikes with Fallout Radionuclide Chronometry","authors":"Joshua D. Landis*, Vivien F. Taylor, Holger Hintelmann and Lee E. Hrenchuk, ","doi":"10.1021/acs.est.4c0154410.1021/acs.est.4c01544","DOIUrl":"https://doi.org/10.1021/acs.est.4c01544https://doi.org/10.1021/acs.est.4c01544","url":null,"abstract":"Soils accumulate anthropogenic mercury (Hg) from atmospheric deposition to terrestrial ecosystems. However, possible reemission of gaseous elemental mercury (GEM) back to the atmosphere as well as downward migration of Hg with soil leachate influence soil sequestration of Hg in ways not sufficiently understood in global biogeochemical models. Here, we apply fallout radionuclide (FRN) chronometry to understand soil Hg dynamics by revisiting the METAALICUS experiments 20 years after enriched isotope tracers (198Hg, 200Hg, 201Hg, and 202Hg) were applied to two boreal watersheds in northwestern Ontario, Canada. Hg spikes formed well-defined peaks in organic horizons of both watersheds at depths of 3–6 cm and were accurately dated to the year of spike application in 6 of 7 cases (error = −0.8 ± 1.2 years). A seventh site was depleted by ca. 90% of both the 200Hg spike and background Hg, and the spike was dated 16 years older than its application. Robust FRN age models and mass balances demonstrate that loss of Hg is attributable to its specific physicochemical behavior at this site, but more work is required to attribute this to reemission or leaching. This study demonstrates the potential of FRN chronometry to provide insights into Hg accumulation, mobilization, and fate in forest soils.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20009–20018 20009–20018"},"PeriodicalIF":10.8,"publicationDate":"2024-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608036","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}

引用次数: 0

Waste Nitrogen Upcycling to Amino Acids during Anaerobic Fermentation on Biochar: An Active Strategy for Regulating Metabolic Reducing Power 生物炭厌氧发酵过程中的废氮转化为氨基酸：调节代谢还原力的主动策略

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-11-01 DOI: 10.1021/acs.est.4c0889010.1021/acs.est.4c08890

Yanfei Tang, Eakalak Khan* and Daniel C. W. Tsang*,

{"title":"Waste Nitrogen Upcycling to Amino Acids during Anaerobic Fermentation on Biochar: An Active Strategy for Regulating Metabolic Reducing Power","authors":"Yanfei Tang, Eakalak Khan* and Daniel C. W. Tsang*, ","doi":"10.1021/acs.est.4c0889010.1021/acs.est.4c08890","DOIUrl":"https://doi.org/10.1021/acs.est.4c08890https://doi.org/10.1021/acs.est.4c08890","url":null,"abstract":"This study proposes a novel strategy that utilizes biochar (BC) during anaerobic fermentation (AF) to generate amino acids (AAs) toward nitrogen upcycling. The BC, pyrolyzed at 800 °C (BC800) to enhance graphite structures and electron-accepting sites, effectively addresses issues related to biosynthetic reducing power nicotinamide adenine dinucleotide phosphate insufficiency by altering cellular conditions and alleviates feedback inhibition through the immobilization of end products. This process establishes unique microbial signaling and energy networks, with Escherichia coli becoming dominant in the biofilm. The conversion rate of ammonia-N to AAs-N within the biofilm reached 67.4% in BC800-AF, which was significantly higher compared to the levels in other AF reactors with BC pyrolyzed at 600 and 400 °C (45.9 and 22.5%, respectively), as well as a control AF reactor (<5%). Furthermore, in BC800-AF, the aromatic AAs (Aro-AAs) were as high as 70.8% of the AAs within the biofilm. The activities of key enzymes for Aro-AAs biosynthesis uniquely positively correlated with the electron-accepting capacity on BC800 (R2 ≥ 0.95). These findings hold promise for transforming existing AF reactors into factories that produce BC-based AAs, providing a more sustainable fertilizing agent than chemical fertilizers.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20060–20072 20060–20072"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608348","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}

引用次数: 0