ACS Applied Polymer Materials最新文献_第7页

Enzymatic Preparation of Machine-Washable Antibacterial Wool through a Subtraction-Addition Technique Using Hydrolase and Transglutaminase 利用水解酶和转谷氨酰胺酶，通过减法添加技术酶解制备机洗抗菌羊毛

IF 7.1 2区化学

ACS Applied Polymer Materials Pub Date : 2024-10-23 DOI: 10.1021/acssuschemeng.4c0777410.1021/acssuschemeng.4c07774

Zirong Li, Kun Li, JiaQi Zhang, Jun Wang, Man Zhou, Yuanyuan Yu, Qiang Wang and Ping Wang*,

{"title":"Enzymatic Preparation of Machine-Washable Antibacterial Wool through a Subtraction-Addition Technique Using Hydrolase and Transglutaminase","authors":"Zirong Li, Kun Li, JiaQi Zhang, Jun Wang, Man Zhou, Yuanyuan Yu, Qiang Wang and Ping Wang*, ","doi":"10.1021/acssuschemeng.4c0777410.1021/acssuschemeng.4c07774","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c07774https://doi.org/10.1021/acssuschemeng.4c07774","url":null,"abstract":"Enzymatic antifelting finishing, as an eco-alternative for conventional chlorination, has attracted increasing attention in wool processing. Nevertheless, proteases are often subject to the disadvantage of significant fiber damage, which is mainly due to the hydrolysis of low-crystallinity cell membrane complexes rather than wool scales. Herein, a full enzymatic subtraction-addition approach was applied to the antifelting finishing of wool textiles, that is, the enzymatic hydrolysis of the highly cross-linked wool scales was carried out by using the hydrolases of keratinase and protease, and then, a glutamine-modified ε-poly-l-lysine (mPLL) was grafted to wool fibers under the catalysis of transglutaminase for enhancing the antifelting effect. According to the test standard of IWS-31, the shrinkage rate of the obtained wool fabric was reduced to 2.98%, and the strength loss was less than 10%, accompanied with encouraging antibacterial activities against Staphylococcus aureus and Escherichia coli, both reaching 100% of antibacterial rates after contact with the bacteria. Meanwhile, low-temperature dyeing can be achieved by enzymatically reducing the density of wool scales, and the mPLL network formed on the wool surface ensures a satisfactory colorfastness to washing and rubbing up to level 4.5. The present enzymatic subtraction-addition technique provides a green route for the functionalization of wool textiles.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16480–16493 16480–16493"},"PeriodicalIF":7.1,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571209","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Hydrogenolysis of Polyethylene by Metal–Organic Framework Confined Single-Site Ruthenium Catalysts 金属有机框架封闭单位钌催化剂对聚乙烯的氢解作用

IF 7.2 2区化学

ACS Applied Polymer Materials Pub Date : 2024-10-23 DOI: 10.1021/acs.chemmater.4c0218610.1021/acs.chemmater.4c02186

Manav Chauhan, Chhaya Thadhani, Bharti Rana, Poorvi Gupta, Biplab Ghosh and Kuntal Manna*,

{"title":"Hydrogenolysis of Polyethylene by Metal–Organic Framework Confined Single-Site Ruthenium Catalysts","authors":"Manav Chauhan, Chhaya Thadhani, Bharti Rana, Poorvi Gupta, Biplab Ghosh and Kuntal Manna*, ","doi":"10.1021/acs.chemmater.4c0218610.1021/acs.chemmater.4c02186","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02186https://doi.org/10.1021/acs.chemmater.4c02186","url":null,"abstract":"Upcycling polyolefins into value-added hydrocarbons via catalytic hydrogenolysis is challenging due to poor product selectivity, random C–C bond cleavage, and the formation of volatile alkanes. We have developed two isoreticular porous aluminum metal–organic framework (MOF) node-supported mononuclear ruthenium dihydride catalysts (DUT-5-RuH2 and MIL-53-RuH2), which are efficient in the hydrogenolysis of low-density polyethylene (LDPE) at 200 °C into a narrow distribution of liquid hydrocarbons (C8-C24). By systematic tuning of the pore sizes of the MOFs, high yields of desirable liquid alkanes were afforded with varying degrees of branching, achieving 80% selectivity. DUT-5-RuH2 produced a C22-centered bell-shaped alkane distribution with a polyethylene conversion of 98%, while MIL-53-RuH2, being selective for shorter alkanes, produced a C9-centered bell-shaped alkane distribution. Based on our spectroscopic and theoretical studies, the high catalytic activity and selectivity of these MOF catalysts are primarily attributed to the stabilization of single-site mono-RuH2 species at the MOF’s nodes via active-site isolation and the confinement of the active catalytic species within porous MOFs. Theoretical calculations suggest that RuH2-mediated polyolefin C–C bond cleavage primarily occurs via turnover-limiting σ-bond metathesis. This study underscores the significance of MOFs in the rational design of heterogeneous catalysts for the efficient upcycling of plastic waste.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"36 21","pages":"10670–10679 10670–10679"},"PeriodicalIF":7.2,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609064","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Defect-Triggered Reversible Phase Transformation for Boosting Electrochemical Performance of Coordination Polymers 缺陷触发可逆相变，提升配位聚合物的电化学性能

IF 7.2 2区化学

ACS Applied Polymer Materials Pub Date : 2024-10-23 DOI: 10.1021/acs.chemmater.4c0195710.1021/acs.chemmater.4c01957

Yixiu Xu, Chenyu Yang, Yi Man, Xinwen Dou, Xin Xiao, Qiang Xu, Qiang Ju*, Qinghua Liu* and Zhenlan Fang*,

{"title":"Defect-Triggered Reversible Phase Transformation for Boosting Electrochemical Performance of Coordination Polymers","authors":"Yixiu Xu, Chenyu Yang, Yi Man, Xinwen Dou, Xin Xiao, Qiang Xu, Qiang Ju*, Qinghua Liu* and Zhenlan Fang*, ","doi":"10.1021/acs.chemmater.4c0195710.1021/acs.chemmater.4c01957","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c01957https://doi.org/10.1021/acs.chemmater.4c01957","url":null,"abstract":"Coordination polymers (CPs) hold promise for reliable and powerful supercapacitors (SCs) to overcome the energy crisis. However, CP-SCs face the daunting challenge of maintaining high pseudocapacitance after long-term charge/discharge cycling. Generally, if introducing defects exerted a positive effect on the property, eliminating defects would show a negative effect, and vice versa. Contrary to this common sense, here we demonstrate that both implanting defects and eliminating defects can significantly boost the specific capacitance of the defect-engineered CPs (DECPs), which are about 1.23 and 1.62 times that of the pristine CP, respectively, without loss of rate capability even after 10,000 charge–discharge cycles. The aqueous (A-ASC) and solid-state asymmetric supercapacitor (SS-ASC) devices based on DECPs deliver high energy densities of 80.3 and 61.5 Wh kg–1, superb power densities of 8471.0 and 8430.6 W kg–1, and long cycling lifespan of up to 2000 cycles with 92.0 and 80.0% capacity retention, respectively. Moreover, the SS-ASC exhibits excellent flexibility, verified by 99.0% maintenance of its initial capacitance when it is twisted and bent at 180°. Importantly, this work has certified that stepwise increasing/decreasing the concentration of ordered defects gradually triggered reversible phase transformation of CP from nonporous to microporous by charge–discharge cycling, in situ addition of the modulator, and postsynthetic treatment. The mechanism of forming/eliminating defects and their effects on supercapacitive performances of CP-SCs have been unprecedentedly clarified. These findings offer insight into the relationship between defective structure and electrochemical behavior for developing efficient long-cycling CP-SCs.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"36 21","pages":"10583–10594 10583–10594"},"PeriodicalIF":7.2,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609224","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Cooperative Transport of Lithium in Disordered Li10MP2S12 (M = Sn, Si) Electrolytes for Li-Ion Batteries 用于锂离子电池的无序 Li10MP2S12（M = Sn，Si）电解质中锂的协同传输

IF 7.2 2区化学

ACS Applied Polymer Materials Pub Date : 2024-10-23 DOI: 10.1021/acs.chemmater.4c0179110.1021/acs.chemmater.4c01791

Vinay Maithani, Sumantra Das and Sankha Mukherjee*,

{"title":"Cooperative Transport of Lithium in Disordered Li10MP2S12 (M = Sn, Si) Electrolytes for Li-Ion Batteries","authors":"Vinay Maithani, Sumantra Das and Sankha Mukherjee*, ","doi":"10.1021/acs.chemmater.4c0179110.1021/acs.chemmater.4c01791","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c01791https://doi.org/10.1021/acs.chemmater.4c01791","url":null,"abstract":"Disorder in sulfide solid-state electrolytes significantly impacts chemical bonding, affecting electrochemical properties and interface stability. Li10GeP2S12, a prominent sulfide electrolyte, is expensive and has limited interfacial stability, so substituting Ge with earth-abundant elements, such as Sn and Si, could be more practical. However, a thorough understanding of the kinetics and chemical bonding nature of Li in the Sn/Si-substituted systems is missing owing to the complexity associated with disordered sublattice in these materials. We use isothermal–isobaric ensemble Car–Parrinello molecular dynamics to evaluate configuration-dependent tracer and charged diffusivities and activation energies for lithium-ion migration in disordered configurations of Li10SiP2S12 (LSiPS) and Li10SnP2S12 (LSnPS) obtained using ensemble statistics. The study uses Li-ion probability density and maximally localized Wannier orbital analysis to determine how temperature and Sn and Si cations affect Li-ion migration. Our findings indicate that higher temperatures enhance Li-ion mobility by enabling more diffusion pathways. The disordered LSiPS and LSnPS electronic structure shows a Kohn–Sham band gap of 2.4 eV for LSiPS and 2 eV for LSnPS, of the most probable configuration across 500 configurations, suggesting a wider electrolyte window for LSiPS. Additionally, Wannier function visualizations demonstrated the significant impact of locality and temperature on the dynamic nature of bonding states of migrating Li ions.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"36 21","pages":"10537–10551 10537–10551"},"PeriodicalIF":7.2,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608767","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Surface Restructuring of Hollow Ni@S-1 Promoted the Activation of CH4 and CO2 in Chemical Looping 中空 Ni@S-1 的表面重组促进了化学循环中 CH4 和 CO2 的活化

IF 7.1 2区化学

ACS Applied Polymer Materials Pub Date : 2024-10-23 DOI: 10.1021/acssuschemeng.4c0448110.1021/acssuschemeng.4c04481

Shuaishuai Meng, Yuhao Wang*, Kongzhai Li, Hua Wang and Yane Zheng*,

{"title":"Surface Restructuring of Hollow Ni@S-1 Promoted the Activation of CH4 and CO2 in Chemical Looping","authors":"Shuaishuai Meng, Yuhao Wang*, Kongzhai Li, Hua Wang and Yane Zheng*, ","doi":"10.1021/acssuschemeng.4c0448110.1021/acssuschemeng.4c04481","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c04481https://doi.org/10.1021/acssuschemeng.4c04481","url":null,"abstract":"Chemical looping reforming of CH4 coupled with the reduction of CO2 is an effective technology for syngas production and CO2 utilization. This work focuses on the surface restructuring of hollow Ni@S-1, which combines with LaFe0.8Co0.15Cu0.05O3 perovskite oxides to obtain a highly efficient oxygen carrier for chemical looping. Ni-impregnated silicalite-1 was subjected to treatment with tetrapropylammonium hydroxide, resulting in the formation of Ni@S-1 with a hollow structure using the “dissolution-recrystallization” method. Nickel is initially present in the form of nickel phyllosilicate in Ni@S-1. After CH4 oxidation, nickel phyllosilicates are transformed into Ni particles that are encapsulated into S-1, effectively suppressing the sintering of Ni particles. In the CH4 oxidation stage, the syngas yield over the LFCC/15%Ni@S-1 decreases slightly from 8.25 to 7.84 mmol·g–1 during 20 redox cycles, demonstrating better stability and reactivity than that of pure LFCC. After 20 redox cycles, Fe and Co elements migrate from perovskite to Ni@S-1, indicating a stronger interaction between perovskite and Ni@S-1, which may benefit the reactivity.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16175–16185 16175–16185"},"PeriodicalIF":7.1,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571148","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Eco-Friendly Antioxidants in Sustainable Biopolymers: A Review 可持续生物聚合物中的生态友好型抗氧化剂：综述

IF 7.1 2区化学

ACS Applied Polymer Materials Pub Date : 2024-10-23 DOI: 10.1021/acssuschemeng.4c0568910.1021/acssuschemeng.4c05689

Shuyi Chen, Jianxiang Feng* and Yuejun Liu,

{"title":"Eco-Friendly Antioxidants in Sustainable Biopolymers: A Review","authors":"Shuyi Chen, Jianxiang Feng* and Yuejun Liu, ","doi":"10.1021/acssuschemeng.4c0568910.1021/acssuschemeng.4c05689","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c05689https://doi.org/10.1021/acssuschemeng.4c05689","url":null,"abstract":"The emergence of eco-friendly antioxidants has gained prominence in recent studies since there is a growing interest in exploring the conversion of traditional synthetic antioxidants into environmentally sustainable additives, which prompts the consideration of more sustainable approaches in the development of new additives. In addition to possessing antioxidant capabilities comparable to synthetic antioxidants, they also have the benefits of being readily accessible, cost-effective, minimally poisonous, and possessing adjustable qualities. Furthermore, the production of sustainable biopolymers is expected to experience significant growth in the future, driven by the desire for a more sustainable economy and less reliance on fossil resources. Fully biobased formulations combining green additives and biopolymers are attracting significant attention in both academia and industry due to the unique benefits of lower carbon emissions and higher biochar content. This review examines four extensively studied categories of eco-friendly antioxidants (natural antioxidants, antioxidants derived from agricultural/food processing industry byproducts, biobased modified antioxidants, and carbon dots of plant origin), including production processes, antioxidant efficiencies, other common performance parameters, and their comparisons with conventional antioxidants; it provides a comprehensive overview and comparative analysis of the sources and properties of these antioxidants, as well as their potential applications in conjunction with sustainable biopolymers in the domains of active food packaging materials, cosmetic products, and biomedical materials. Furthermore, the obstacles and potential opportunities associated with developing eco-friendly antioxidants are summarized.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16126–16145 16126–16145"},"PeriodicalIF":7.1,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571215","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Synthesis and Evaluation of Polymer-Drug Conjugates as Potential Antioxidants and Cholinesterase Inhibitors for Neurodegenerative Diseases 合成和评估聚合物-药物共轭物作为神经退行性疾病的潜在抗氧化剂和胆碱酯酶抑制剂

IF 7.2 2区化学

ACS Applied Polymer Materials Pub Date : 2024-10-23 DOI: 10.1021/acs.chemmater.4c0176710.1021/acs.chemmater.4c01767

Nuruddin Mahadik, Gemma A. Barron, Paul Kong Thoo Lin and Colin J. Thompson*,

{"title":"Synthesis and Evaluation of Polymer-Drug Conjugates as Potential Antioxidants and Cholinesterase Inhibitors for Neurodegenerative Diseases","authors":"Nuruddin Mahadik, Gemma A. Barron, Paul Kong Thoo Lin and Colin J. Thompson*, ","doi":"10.1021/acs.chemmater.4c0176710.1021/acs.chemmater.4c01767","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c01767https://doi.org/10.1021/acs.chemmater.4c01767","url":null,"abstract":"Polymer-drug conjugates (PDCs) may offer improved water-solubility and in vitro activity of potential antioxidant and cholinesterase (ChE) inhibitor drugs compared to the drugs alone. Conjugation of these potential drugs to water-soluble polymers could increase their therapeutic efficacy. Vanillin was conjugated to poly(allylamine hydrochloride) (NM10 and NM15) and naphthalimidohexylamine (HEXNAP) was conjugated to poly(acrylic acid) (N5 and N10). The antioxidant and cholinesterase inhibitory activities of these novel PDCs were evaluated and compared with those of their respective starting materials. Additionally, in silico molecular modeling studies were conducted to explore the potential cholinesterase inhibitory mechanisms of these conjugates. NM15 (unadjusted and adjusted value) showed significantly enhanced in vitro antioxidant activity (p ≤ 0.0001) compared to vanillin. The adjusted value of N5 compared to HEXNAP showed significantly enhanced in vitro cholinesterase inhibitory activity against acetylcholinesterase (AChE) and butyrylcholinesterase (BuChE) (p ≤ 0.0001). Kinetic and molecular modeling studies revealed that N5 was a competitive inhibitor of butyrylcholinesterase and interacted with the active sites of human acetylcholinesterase and human butyrylcholinesterase enzymes. NM15 and N5 were identified as lead PDCs based on their enhanced antioxidant and cholinesterase inhibitory activity, respectively. Overall, this work demonstrates the potential use of PDCs as treatment options for neurodegenerative diseases.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"36 21","pages":"10514–10527 10514–10527"},"PeriodicalIF":7.2,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemmater.4c01767","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609223","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

First Photocatalytic Synthesis of Cyclic Carbonates from CO2 Using Bromide-Functionalized Polyoxometalate without Additional Cocatalyst 利用溴化物官能化聚氧金属铝酸盐首次光催化合成二氧化碳环碳酸盐，无需额外的催化剂

IF 7.1 2区化学

ACS Applied Polymer Materials Pub Date : 2024-10-23 DOI: 10.1021/acssuschemeng.4c0667610.1021/acssuschemeng.4c06676

Huafeng Li*, Hui Kong, Jianzhong Guo, Bing Li, Shanshan Zhang, Suzhi Li, Junwei Zhao* and Liqun Bai*,

{"title":"First Photocatalytic Synthesis of Cyclic Carbonates from CO2 Using Bromide-Functionalized Polyoxometalate without Additional Cocatalyst","authors":"Huafeng Li*, Hui Kong, Jianzhong Guo, Bing Li, Shanshan Zhang, Suzhi Li, Junwei Zhao* and Liqun Bai*, ","doi":"10.1021/acssuschemeng.4c0667610.1021/acssuschemeng.4c06676","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c06676https://doi.org/10.1021/acssuschemeng.4c06676","url":null,"abstract":"Developing photocatalysts with low energy consumption and high efficiency for CO2 fixation without any cocatalyst is a highly sought-after goal, but it still presents a significant challenge. Herein, aiming at enhancing the efficiency of photodriven CO2 cycloaddition reactions, an imidazolium bromide ionic liquid-functionalized polyoxometalate photocatalyst ImBr-[Ru(C10N2H8)2]H[AsW12O40]·2H2O with Ru-based photosensitizer coordinated with ionic liquids via strong coupling between the metal active site and carboxy group is reported. The optimized ImBr-[Ru(C10N2H8)2]H[AsW12O40]·2H2O achieves efficient photocatalytic CO2 cycloaddition with epoxides at ambient temperature without additional cocatalyst and photosensitizer, which is much higher than most reported photocatalysts in the presence of TBAB cocatalyst. The experimental results indicated that imidazolium bromide ionic liquid facilitating the ring-opened reaction of epoxides, the radical mechanism, and a plausible reaction pathway for the epoxidation step was further proposed by in situ DRIFT and EPR. Remarkably, this is the first report on the photoeffect of polyoxometalate-based catalysts with ionic liquid-functionalized molecules for catalytic CO2 photofixation without any cocatalyst and sacrificial agent.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16396–16408 16396–16408"},"PeriodicalIF":7.1,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571213","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Heavy Metal-Resistant Biohybrid System Boosts Dissimilatory Nitrate Reduction to Ammonium for Agronomic Sustainability 抗重金属生物杂交系统促进硝酸盐分解为氨，实现农艺可持续性

IF 7.1 2区化学

ACS Applied Polymer Materials Pub Date : 2024-10-23 DOI: 10.1021/acssuschemeng.4c0716610.1021/acssuschemeng.4c07166

Jialin Chi, Shiyin Wu, Liping Fang, Kai Liu, Shaochen Huang, Wenjun Zhang and Fangbai Li*,

{"title":"Heavy Metal-Resistant Biohybrid System Boosts Dissimilatory Nitrate Reduction to Ammonium for Agronomic Sustainability","authors":"Jialin Chi, Shiyin Wu, Liping Fang, Kai Liu, Shaochen Huang, Wenjun Zhang and Fangbai Li*, ","doi":"10.1021/acssuschemeng.4c0716610.1021/acssuschemeng.4c07166","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c07166https://doi.org/10.1021/acssuschemeng.4c07166","url":null,"abstract":"Dissimilatory nitrate reduction to ammonium (DNRA) by functional microbes is crucial for optimizing nitrogen preservation and sustainable utilization in agricultural soils, particularly in paddy soils where nitrogen management is essential for crop yields, while the biocatalytic efficiency for this process is always limited, especially in soils polluted with heavy metals such as cadmium (Cd). In this study, we strategically designed a heavy metal-resistant nanogel (Bg) material with variable functional groups incorporating imidazole, carboxyl, and thiol groups and hybridized this material with DNRA functional strain, Shewanella oneidensis MR-1, resulting in a biohybrid system. Notably, the biohybrid system efficiently catalyzed DNRA processes, achieving up to around 2–4 times increase in nitrogen transformation rates in the absence/presence of Cd2+ compared to S. oneidensis MR-1 alone because the Bg material from the biohybrid system can promote DNRA by functional strain and mediate Cd immobilization processes through distinct functional groups. Within the biohybrid-mediated DNRA process, the thiol groups derived from Bg act as electron shuttles, significantly promoting the extent and rate of DNRA. For the Cd immobilization process, the imidazole and carboxyl groups within Asp-xxx-His sequences from Bg serve as primary Cd binding sites, as confirmed by dynamic force spectroscopy (DFS). This study provides valuable insights into the precise control of nitrogen cycling and sustainable utilization in agricultural soils, highlighting the significant role of the designed biohybrid materials in enhancing both DNRA efficiency and heavy metal immobilization.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16444–16452 16444–16452"},"PeriodicalIF":7.1,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571085","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Manganese-Biochar Catalyst for Sustainable Glycolic Acid Production from Biomass-Derived Glucose and Oligosaccharides 利用生物质提取的葡萄糖和低聚糖生产可持续乙醇酸的锰-生物炭催化剂

IF 7.1 2区化学

ACS Applied Polymer Materials Pub Date : 2024-10-23 DOI: 10.1021/acssuschemeng.4c0693810.1021/acssuschemeng.4c06938

Qiaozhi Zhang, Yang Cao, Zibo Xu, Hanwu Lei, Xiaoguang Duan, James H. Clark and Daniel C. W. Tsang*,

{"title":"Manganese-Biochar Catalyst for Sustainable Glycolic Acid Production from Biomass-Derived Glucose and Oligosaccharides","authors":"Qiaozhi Zhang, Yang Cao, Zibo Xu, Hanwu Lei, Xiaoguang Duan, James H. Clark and Daniel C. W. Tsang*, ","doi":"10.1021/acssuschemeng.4c0693810.1021/acssuschemeng.4c06938","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c06938https://doi.org/10.1021/acssuschemeng.4c06938","url":null,"abstract":"Production of glycolic acid from renewable resources is a significant challenge considering its extensive market and the depletion of fossil resources. This study accomplished sustainable glycolic acid production from biomass-derived saccharides using a microwave-assisted aerobic oxidation system. Various Mn-biochar catalysts were synthesized using different precursors (MnCl2 and KMnO4) and synthesis temperatures (400–850 °C). Glycolic acid yield from glucose could reach 62.8 Cmol % within 20 min at 180 °C over MnBC-VII-700 (i.e., catalyst derived from Mn(VII) precursor and synthesized at 700 °C). Mn(III) was identified as the catalytically active state by correlation with the catalytic performance. Biochar support is vital for reactant adsorption, electron transfer, and microwave absorption. Transformation from glucose to glycolic acid would experience retro-aldol and oxidation reactions, while oxidation-hydrolysis of the glycosidic bond could be achieved for one-pot oligosaccharide conversion. The yields of glycolic acid reached 43.1, 29.2, and 33.3 Cmol % within 30 min, when the substrates were cellobiose, maltose, and maltotriose, respectively. This study developed a low-cost Mn-biochar catalyst for biomass valorization. The study presents valuable mechanistic insights that can serve as a critical reference for the sustainable production of chemical building blocks in heterogeneous catalysis.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"12 44","pages":"16423–16433 16423–16433"},"PeriodicalIF":7.1,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571208","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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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