ACS Sustainable Chemistry & Engineering最新文献_第9页

Nanostructured Copper@Carbon Fiber Composite as an Advanced Anode Catalyst in High-Performance Aqueous Viologen Flow Batteries 纳米结构Copper@Carbon纤维复合材料作为高性能水凝胶液流电池的高级阳极催化剂

IF 8.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering

Pub Date : 2026-01-27 DOI: 10.1021/acssuschemeng.5c12173

Ruoqing Sun, Guanghui Zhou, Ying Liu, Haiguang Gao, Juan Xu, Jianyu Cao, Yonggang Wang

Redox flow batteries (RFBs) are a promising technology for large-scale energy storage due to their decoupled power and energy architecture, high scalability, and safety. Redox-active organic materials (ROMs) have emerged as promising candidates for RFB applications due to their molecular diversity, structural flexibility, cost effectiveness, and environmental compatibility. However, the sluggish kinetics of promising ROMs like methyl viologen (MV) on conventional carbon felt (CF) electrodes remain a critical bottleneck, necessitating the development of highly active electrocatalysts. Herein, we report the development of a novel nanostructured copper-on-carbon-felt composite (Cu@CF) electrode fabricated via a facile electrodeposition method incorporating organic additives. The Cu@CF electrode significantly enhances the intrinsic kinetic rate constant (k⁰) of the MV redox reaction by approximately 3-fold compared to that of pristine CF, demonstrating its superior intrinsic catalytic capability. An MV//N,N,N-2,2,6,6-heptamethylpiperidinyl-oxy-4-ammonium (TEMPTMA) aqueous organic redox flow battery (AORFB) full cell assembled using Cu@CF as the anode catalyst demonstrates substantially enhanced performance metrics, including remarkably low area-specific resistance (ASR), higher discharge capacity (85.1% utilization at 30 mA cm^–2), a maximum power density of 235.4 mW cm^–2 (46% higher than the CF cell), and excellent energy efficiency (EE) of 79.7% at 80 mA cm^–2. Furthermore, this Cu@CF cell exhibits superior long-term stability over 500 cycles, maintaining an average EE of 78.52% and effectively suppressing undesirable side reactions like dimerization and disproportionation of MV^+• (the reduced state of MV²⁺). This work establishes Cu@CF as a high-performance, durable, and low-cost electrocatalyst, offering a practical strategy to advance viologen-based AORFB technology.

氧化还原液流电池（rfb）由于其解耦的功率和能量结构、高可扩展性和安全性，是一种很有前途的大规模储能技术。氧化还原活性有机材料（ROMs）由于其分子多样性、结构灵活性、成本效益和环境相容性而成为RFB应用的有希望的候选者。然而，像甲基紫素（MV）这样有前途的rom在传统碳毡（CF）电极上的缓慢动力学仍然是一个关键的瓶颈，需要开发高活性的电催化剂。在此，我们报告了一种新型纳米结构碳上铜毡复合材料（Cu@CF）电极的开发，该电极通过结合有机添加剂的简易电沉积方法制造。Cu@CF电极显著提高了MV氧化还原反应的本然动力学速率常数k0，比原始CF提高了约3倍，显示了其优越的本然催化能力。使用Cu@CF作为阳极催化剂组装的MV//N，N,N-2,2,6,6-七甲基piperidyl -氧-4-铵（TEMPTMA）水相有机氧化还原液流电池（AORFB）全电池表现出显著增强的性能指标，包括极低的面积比电阻（ASR），更高的放电容量（30 mA cm-2时利用率为85.1%），最大功率密度为235.4 mW cm-2（比CF电池高46%），以及80 mA cm-2时79.7%的优异能效（EE）。此外，这种Cu@CF电池在500次循环中表现出优异的长期稳定性，保持78.52%的平均EE，并有效抑制MV+•（MV2+的还原状态）的二聚化和歧化等不良副反应。这项工作确立了Cu@CF作为一种高性能、耐用、低成本的电催化剂，为推进基于viologen的AORFB技术提供了一种实用的策略。

{"title":"Nanostructured Copper@Carbon Fiber Composite as an Advanced Anode Catalyst in High-Performance Aqueous Viologen Flow Batteries","authors":"Ruoqing Sun, Guanghui Zhou, Ying Liu, Haiguang Gao, Juan Xu, Jianyu Cao, Yonggang Wang","doi":"10.1021/acssuschemeng.5c12173","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c12173","url":null,"abstract":"Redox flow batteries (RFBs) are a promising technology for large-scale energy storage due to their decoupled power and energy architecture, high scalability, and safety. Redox-active organic materials (ROMs) have emerged as promising candidates for RFB applications due to their molecular diversity, structural flexibility, cost effectiveness, and environmental compatibility. However, the sluggish kinetics of promising ROMs like methyl viologen (MV) on conventional carbon felt (CF) electrodes remain a critical bottleneck, necessitating the development of highly active electrocatalysts. Herein, we report the development of a novel nanostructured copper-on-carbon-felt composite (Cu@CF) electrode fabricated via a facile electrodeposition method incorporating organic additives. The Cu@CF electrode significantly enhances the intrinsic kinetic rate constant (k0) of the MV redox reaction by approximately 3-fold compared to that of pristine CF, demonstrating its superior intrinsic catalytic capability. An MV//N,N,N-2,2,6,6-heptamethylpiperidinyl-oxy-4-ammonium (TEMPTMA) aqueous organic redox flow battery (AORFB) full cell assembled using Cu@CF as the anode catalyst demonstrates substantially enhanced performance metrics, including remarkably low area-specific resistance (ASR), higher discharge capacity (85.1% utilization at 30 mA cm–2), a maximum power density of 235.4 mW cm–2 (46% higher than the CF cell), and excellent energy efficiency (EE) of 79.7% at 80 mA cm–2. Furthermore, this Cu@CF cell exhibits superior long-term stability over 500 cycles, maintaining an average EE of 78.52% and effectively suppressing undesirable side reactions like dimerization and disproportionation of MV+• (the reduced state of MV2+). This work establishes Cu@CF as a high-performance, durable, and low-cost electrocatalyst, offering a practical strategy to advance viologen-based AORFB technology.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"10 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089919","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

Chemical Upcycling of Waste Chlorinated Plastics into α,ω-Dienes via Consecutive Dehydrochlorination-Hydrogenation with HCl Trapping and Metathesis 氯化废塑料连续脱氢-加氢- HCl捕集-复分解化学回收制备α，ω-二烯

IF 7.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering

Pub Date : 2026-01-26 DOI: 10.1021/acssuschemeng.5c11948

Christophe Vos, , , Galahad O’Rourke, , and , Dirk De Vos*,

The chemical recycling of chlorinated plastics is industrially challenging due to the release of corrosive HCl and char formation. In this work, a novel upcycling route for chlorinated plastics, including polyvinyl chloride (PVC), polyvinylidene chloride (PVDC), and chlorinated polyethylene (CPE), is developed. When ZnCl₂-catalyzed dehydrochlorination (DHC) is combined with tandem DHC-hydrogenation, using a homogeneous Ru hydrogenation catalyst and metal oxides as a HCl trap, each plastic type can be selectively converted into an unsaturated polyolefin (UPO), which can be chemically split via metathesis. By rational design of reaction conditions, CPE (25 or 35 m% Cl) as a model substrate, a PVDC–PVC copolymer (66 m% Cl) and PVC (57 m% Cl) were consecutively converted into partially and fully dechlorinated UPOs. Both of these UPO products contained −CH₂–CH₂–sequences and up to 11 double bonds per 100 carbons. They were chemically split into α,ω-dienes using a second-generation Grubbs catalyst. Via this procedure, chlorinated plastics can be converted into valuable chemical building blocks, while the released HCl is sequestered.

氯化塑料的化学回收是工业上具有挑战性的，因为释放腐蚀性的HCl和炭的形成。在这项工作中，开发了一种新的氯化塑料升级回收途径，包括聚氯乙烯（PVC），聚偏氯乙烯（PVDC）和氯化聚乙烯（CPE）。当zncl2催化脱氢氯化（DHC）与DHC-串列加氢相结合，使用均相Ru加氢催化剂和金属氧化物作为HCl陷阱时，每种塑料类型都可以选择性地转化为不饱和聚烯烃（UPO）， UPO可以通过化学分解进行化学分裂。通过合理设计反应条件，以CPE（25或35 m% Cl）为模型底物，分别将PVC - PVC共聚物（66 m% Cl）和PVC （57 m% Cl）分别转化为部分脱氯和完全脱氯的upo。这两种UPO产物都含有−ch2 - ch2序列，每100个碳上含有多达11个双键。利用第二代格拉布催化剂，它们被化学分解成α，ω-二烯。通过这一过程，氯化塑料可以转化为有价值的化学构件，而释放的HCl被隔离。

{"title":"Chemical Upcycling of Waste Chlorinated Plastics into α,ω-Dienes via Consecutive Dehydrochlorination-Hydrogenation with HCl Trapping and Metathesis","authors":"Christophe Vos, , , Galahad O’Rourke, , and , Dirk De Vos*, ","doi":"10.1021/acssuschemeng.5c11948","DOIUrl":"10.1021/acssuschemeng.5c11948","url":null,"abstract":"The chemical recycling of chlorinated plastics is industrially challenging due to the release of corrosive HCl and char formation. In this work, a novel upcycling route for chlorinated plastics, including polyvinyl chloride (PVC), polyvinylidene chloride (PVDC), and chlorinated polyethylene (CPE), is developed. When ZnCl2-catalyzed dehydrochlorination (DHC) is combined with tandem DHC-hydrogenation, using a homogeneous Ru hydrogenation catalyst and metal oxides as a HCl trap, each plastic type can be selectively converted into an unsaturated polyolefin (UPO), which can be chemically split via metathesis. By rational design of reaction conditions, CPE (25 or 35 m% Cl) as a model substrate, a PVDC–PVC copolymer (66 m% Cl) and PVC (57 m% Cl) were consecutively converted into partially and fully dechlorinated UPOs. Both of these UPO products contained −CH2–CH2–sequences and up to 11 double bonds per 100 carbons. They were chemically split into α,ω-dienes using a second-generation Grubbs catalyst. Via this procedure, chlorinated plastics can be converted into valuable chemical building blocks, while the released HCl is sequestered.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"14 5","pages":"2595–2605"},"PeriodicalIF":7.3,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044927","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

Microwave Electrification as a Process-Intensification Strategy for Calcination-Free, Scalable, and Sustainable Synthesis of Anatase-TiO2/α-Fe2O3 Photocatalysts 微波电气化作为无煅烧、可扩展和可持续合成锐钛矿- tio2 /α-Fe2O3光催化剂的工艺强化策略

IF 8.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering

Pub Date : 2026-01-26 DOI: 10.1021/acssuschemeng.5c12003

Praveen Kumar Lavudya,Sesha SuryaBindu Devarakonda,Dharani Kumar Chennamsetty,Nowduru Ravikiran,Venkata Satya Siva Srikanth Vadali,Rajanikanth Ammanabrolu

While anatase-TiO2/α-Fe2O3 (ATAF) composites are promising visible-light photocatalysts, their conventional synthesis is hindered by prolonged processing and high-temperature calcination, which limits scalability and increases energy consumption. This work demonstrates a rapid, single-step microwave-hydrothermal strategy to fabricate phase-pure ATAF composites within 10 min, entirely without calcination. This method facilitates the heterogeneous nucleation of anatase-TiO2 onto α-Fe2O3 particles, creating an intimate interface. By optimizing the α-Fe2O3 content with uniform TiO2 decoration on it, an ATAF composite exhibiting superior charge separation, as evidenced by significant photoluminescence quenching, is prepared. This optimal interface engineering results in a remarkable 99.9% photocatalytic degradation of methylene blue under visible light, significantly outperforming the individual constituents. This energy-efficient approach potentially reduces synthesis energy consumption by one to 2 orders of magnitude compared to conventional calcination routes, while the use of aqueous solvents and a closed system aligns with the principles of clean production. The combined advantages of rapid processing, energy efficiency, and scalability position this method as a viable pathway for the industrial-scale production of high-performance photocatalytic composites. The microwave-assisted hydrothermal synthesis demonstrates process electrification by transitioning from conventional furnace-based thermal treatment to direct microwave heating, resulting in reduced energy consumption and associated CO2 emissions.

虽然锐钛矿- tio2 /α-Fe2O3 （ATAF）复合材料是很有前途的可见光催化剂，但其传统合成受到长时间加工和高温煅烧的阻碍，这限制了可扩展性并增加了能耗。这项工作展示了一种快速的单步微波热液策略，可以在10分钟内制造相纯ATAF复合材料，完全不需要煅烧。这种方法有利于锐钛矿- tio2在α-Fe2O3颗粒上的非均相成核，形成一个紧密的界面。通过对α-Fe2O3含量进行优化，并在α-Fe2O3表面均匀修饰，制备出具有良好电荷分离性能的ATAF复合材料，并具有明显的光致猝灭现象。这种优化的界面工程使得亚甲基蓝在可见光下的光催化降解率达到99.9%，显著优于单个组分。与传统的煅烧路线相比，这种节能方法有可能将合成能耗降低一到两个数量级，同时使用水性溶剂和封闭系统符合清洁生产的原则。快速处理、能源效率和可扩展性的综合优势使该方法成为工业规模生产高性能光催化复合材料的可行途径。微波辅助水热合成证明了工艺电气化，从传统的基于炉的热处理过渡到直接微波加热，从而降低了能耗和相关的二氧化碳排放。

{"title":"Microwave Electrification as a Process-Intensification Strategy for Calcination-Free, Scalable, and Sustainable Synthesis of Anatase-TiO2/α-Fe2O3 Photocatalysts","authors":"Praveen Kumar Lavudya,Sesha SuryaBindu Devarakonda,Dharani Kumar Chennamsetty,Nowduru Ravikiran,Venkata Satya Siva Srikanth Vadali,Rajanikanth Ammanabrolu","doi":"10.1021/acssuschemeng.5c12003","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c12003","url":null,"abstract":"While anatase-TiO2/α-Fe2O3 (ATAF) composites are promising visible-light photocatalysts, their conventional synthesis is hindered by prolonged processing and high-temperature calcination, which limits scalability and increases energy consumption. This work demonstrates a rapid, single-step microwave-hydrothermal strategy to fabricate phase-pure ATAF composites within 10 min, entirely without calcination. This method facilitates the heterogeneous nucleation of anatase-TiO2 onto α-Fe2O3 particles, creating an intimate interface. By optimizing the α-Fe2O3 content with uniform TiO2 decoration on it, an ATAF composite exhibiting superior charge separation, as evidenced by significant photoluminescence quenching, is prepared. This optimal interface engineering results in a remarkable 99.9% photocatalytic degradation of methylene blue under visible light, significantly outperforming the individual constituents. This energy-efficient approach potentially reduces synthesis energy consumption by one to 2 orders of magnitude compared to conventional calcination routes, while the use of aqueous solvents and a closed system aligns with the principles of clean production. The combined advantages of rapid processing, energy efficiency, and scalability position this method as a viable pathway for the industrial-scale production of high-performance photocatalytic composites. The microwave-assisted hydrothermal synthesis demonstrates process electrification by transitioning from conventional furnace-based thermal treatment to direct microwave heating, resulting in reduced energy consumption and associated CO2 emissions.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"51 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044929","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

Chemical Upcycling of Waste Chlorinated Plastics into α,ω-Dienes via Consecutive Dehydrochlorination-Hydrogenation with HCl Trapping and Metathesis 氯化废塑料连续脱氢-加氢- HCl捕集-复分解化学回收制备α，ω-二烯

IF 8.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering

Pub Date : 2026-01-26 DOI: 10.1021/acssuschemeng.5c11948

Christophe Vos,Galahad O’Rourke,Dirk De Vos

The chemical recycling of chlorinated plastics is industrially challenging due to the release of corrosive HCl and char formation. In this work, a novel upcycling route for chlorinated plastics, including polyvinyl chloride (PVC), polyvinylidene chloride (PVDC), and chlorinated polyethylene (CPE), is developed. When ZnCl2-catalyzed dehydrochlorination (DHC) is combined with tandem DHC-hydrogenation, using a homogeneous Ru hydrogenation catalyst and metal oxides as a HCl trap, each plastic type can be selectively converted into an unsaturated polyolefin (UPO), which can be chemically split via metathesis. By rational design of reaction conditions, CPE (25 or 35 m% Cl) as a model substrate, a PVDC–PVC copolymer (66 m% Cl) and PVC (57 m% Cl) were consecutively converted into partially and fully dechlorinated UPOs. Both of these UPO products contained −CH2–CH2–sequences and up to 11 double bonds per 100 carbons. They were chemically split into α,ω-dienes using a second-generation Grubbs catalyst. Via this procedure, chlorinated plastics can be converted into valuable chemical building blocks, while the released HCl is sequestered.

氯化塑料的化学回收是工业上具有挑战性的，因为释放腐蚀性的HCl和炭的形成。在这项工作中，开发了一种新的氯化塑料升级回收途径，包括聚氯乙烯（PVC），聚偏氯乙烯（PVDC）和氯化聚乙烯（CPE）。当zncl2催化脱氢氯化（DHC）与DHC-串列加氢相结合，使用均相Ru加氢催化剂和金属氧化物作为HCl陷阱时，每种塑料类型都可以选择性地转化为不饱和聚烯烃（UPO）， UPO可以通过化学分解进行化学分裂。通过合理设计反应条件，以CPE（25或35 m% Cl）为模型底物，分别将PVC - PVC共聚物（66 m% Cl）和PVC （57 m% Cl）分别转化为部分脱氯和完全脱氯的upo。这两种UPO产物都含有−ch2 - ch2序列，每100个碳上含有多达11个双键。利用第二代格拉布催化剂，它们被化学分解成α，ω-二烯。通过这一过程，氯化塑料可以转化为有价值的化学构件，而释放的HCl被隔离。

{"title":"Chemical Upcycling of Waste Chlorinated Plastics into α,ω-Dienes via Consecutive Dehydrochlorination-Hydrogenation with HCl Trapping and Metathesis","authors":"Christophe Vos,Galahad O’Rourke,Dirk De Vos","doi":"10.1021/acssuschemeng.5c11948","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c11948","url":null,"abstract":"The chemical recycling of chlorinated plastics is industrially challenging due to the release of corrosive HCl and char formation. In this work, a novel upcycling route for chlorinated plastics, including polyvinyl chloride (PVC), polyvinylidene chloride (PVDC), and chlorinated polyethylene (CPE), is developed. When ZnCl2-catalyzed dehydrochlorination (DHC) is combined with tandem DHC-hydrogenation, using a homogeneous Ru hydrogenation catalyst and metal oxides as a HCl trap, each plastic type can be selectively converted into an unsaturated polyolefin (UPO), which can be chemically split via metathesis. By rational design of reaction conditions, CPE (25 or 35 m% Cl) as a model substrate, a PVDC–PVC copolymer (66 m% Cl) and PVC (57 m% Cl) were consecutively converted into partially and fully dechlorinated UPOs. Both of these UPO products contained −CH2–CH2–sequences and up to 11 double bonds per 100 carbons. They were chemically split into α,ω-dienes using a second-generation Grubbs catalyst. Via this procedure, chlorinated plastics can be converted into valuable chemical building blocks, while the released HCl is sequestered.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"40 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044930","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

Increased Giga-Cubic Meters of the Water Footprint of China’s Coal Caused by Washing 洗涤导致中国煤炭水足迹增加千兆立方米

IF 8.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering

Pub Date : 2026-01-26 DOI: 10.1021/acssuschemeng.5c09674

Jie Zhang, Xiaofan Wang, Yirong Wang, Yulong Yan, Sheng Zhang, Lin Peng, Menggang Li, Kechang Xie, Junjie Li

Coal washing plays a vital role in improving coal quality and reducing atmospheric pollutant emissions from coal combustion. However, the water footprint burdens caused by substantial freshwater consumption and wastewater discharge remain poorly understood. In this study, a comprehensive water footprint framework for coal washing was developed and used for a bottom-up analysis based on firsthand data from 2,367 coal washing plants across China in 2022. Compared with the scenario where coal was not washed, the national coal washing industry increases the water footprint by 7.38 Gm³, bringing the total water footprint of China’s coal supply chain to 27.68 Gm³, with gray water accounting for 90.9%. The water footprint intensities of commercial coal varied between 6.93 and 27.33 m³/t depending on the washing technologies, with a national average of 8.73 m³/t. Among the various technologies, jigging and jigging-based combined processes demonstrated relatively low water footprint intensities. From a production perspective, the spatial distribution of water footprint intensities in China exhibits a “high in the south and low in the north” pattern. However, an interprovincial transfer of 12.72 Gm³ of water footprint exacerbated the spatial mismatch between coal resources and water availability, owing to mismatches between production and consumption centers and prevailing trade flows. This study highlights the significant contribution of coal washing to the total water footprint of the coal life cycle and underscores the urgent need to incorporate water footprint balance into policies and decision-making regarding coal washing practices.

洗煤对提高煤质、减少燃煤排放大气污染物具有重要作用。然而，大量淡水消耗和废水排放造成的水足迹负担仍然知之甚少。在这项研究中，基于2022年中国2367家洗煤厂的第一手数据，开发了一个全面的洗煤水足迹框架，并将其用于自下而上的分析。与不洗煤情景相比，全国洗煤行业增加了7.38 Gm3的水足迹，使中国煤炭供应链的总水足迹达到27.68 Gm3，其中灰水占90.9%。商品煤的水足迹强度根据洗选技术的不同在6.93 ~ 27.33 m3/t之间，全国平均为8.73 m3/t。在各种工艺中，跳汰和基于跳汰的组合工艺表现出相对较低的水足迹强度。从生产角度看，中国水足迹强度的空间分布呈现“南高北低”的格局。然而，12.72 Gm3的水足迹跨省转移加剧了煤炭资源与水资源可得性的空间失配，这主要是由于生产和消费中心与主流贸易流之间的失配。这项研究强调了洗煤对煤炭生命周期总水足迹的重大贡献，并强调了将水足迹平衡纳入有关洗煤实践的政策和决策的迫切需要。

{"title":"Increased Giga-Cubic Meters of the Water Footprint of China’s Coal Caused by Washing","authors":"Jie Zhang, Xiaofan Wang, Yirong Wang, Yulong Yan, Sheng Zhang, Lin Peng, Menggang Li, Kechang Xie, Junjie Li","doi":"10.1021/acssuschemeng.5c09674","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c09674","url":null,"abstract":"Coal washing plays a vital role in improving coal quality and reducing atmospheric pollutant emissions from coal combustion. However, the water footprint burdens caused by substantial freshwater consumption and wastewater discharge remain poorly understood. In this study, a comprehensive water footprint framework for coal washing was developed and used for a bottom-up analysis based on firsthand data from 2,367 coal washing plants across China in 2022. Compared with the scenario where coal was not washed, the national coal washing industry increases the water footprint by 7.38 Gm3, bringing the total water footprint of China’s coal supply chain to 27.68 Gm3, with gray water accounting for 90.9%. The water footprint intensities of commercial coal varied between 6.93 and 27.33 m3/t depending on the washing technologies, with a national average of 8.73 m3/t. Among the various technologies, jigging and jigging-based combined processes demonstrated relatively low water footprint intensities. From a production perspective, the spatial distribution of water footprint intensities in China exhibits a “high in the south and low in the north” pattern. However, an interprovincial transfer of 12.72 Gm3 of water footprint exacerbated the spatial mismatch between coal resources and water availability, owing to mismatches between production and consumption centers and prevailing trade flows. This study highlights the significant contribution of coal washing to the total water footprint of the coal life cycle and underscores the urgent need to incorporate water footprint balance into policies and decision-making regarding coal washing practices.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"29 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146048753","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

Microwave Electrification as a Process-Intensification Strategy for Calcination-Free, Scalable, and Sustainable Synthesis of Anatase-TiO2/α-Fe2O3 Photocatalysts 微波电气化作为无煅烧、可扩展和可持续合成锐钛矿- tio2 /α-Fe2O3光催化剂的工艺强化策略

IF 8.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering

Pub Date : 2026-01-26 DOI: 10.1021/acssuschemeng.5c12003

Praveen Kumar Lavudya,Sesha SuryaBindu Devarakonda,Dharani Kumar Chennamsetty,Nowduru Ravikiran,Venkata Satya Siva Srikanth Vadali,Rajanikanth Ammanabrolu

While anatase-TiO2/α-Fe2O3 (ATAF) composites are promising visible-light photocatalysts, their conventional synthesis is hindered by prolonged processing and high-temperature calcination, which limits scalability and increases energy consumption. This work demonstrates a rapid, single-step microwave-hydrothermal strategy to fabricate phase-pure ATAF composites within 10 min, entirely without calcination. This method facilitates the heterogeneous nucleation of anatase-TiO2 onto α-Fe2O3 particles, creating an intimate interface. By optimizing the α-Fe2O3 content with uniform TiO2 decoration on it, an ATAF composite exhibiting superior charge separation, as evidenced by significant photoluminescence quenching, is prepared. This optimal interface engineering results in a remarkable 99.9% photocatalytic degradation of methylene blue under visible light, significantly outperforming the individual constituents. This energy-efficient approach potentially reduces synthesis energy consumption by one to 2 orders of magnitude compared to conventional calcination routes, while the use of aqueous solvents and a closed system aligns with the principles of clean production. The combined advantages of rapid processing, energy efficiency, and scalability position this method as a viable pathway for the industrial-scale production of high-performance photocatalytic composites. The microwave-assisted hydrothermal synthesis demonstrates process electrification by transitioning from conventional furnace-based thermal treatment to direct microwave heating, resulting in reduced energy consumption and associated CO2 emissions.

虽然锐钛矿- tio2 /α-Fe2O3 （ATAF）复合材料是很有前途的可见光催化剂，但其传统合成受到长时间加工和高温煅烧的阻碍，这限制了可扩展性并增加了能耗。这项工作展示了一种快速的单步微波热液策略，可以在10分钟内制造相纯ATAF复合材料，完全不需要煅烧。这种方法有利于锐钛矿- tio2在α-Fe2O3颗粒上的非均相成核，形成一个紧密的界面。通过对α-Fe2O3含量进行优化，并在α-Fe2O3表面均匀修饰，制备出具有良好电荷分离性能的ATAF复合材料，并具有明显的光致猝灭现象。这种优化的界面工程使得亚甲基蓝在可见光下的光催化降解率达到99.9%，显著优于单个组分。与传统的煅烧路线相比，这种节能方法有可能将合成能耗降低一到两个数量级，同时使用水性溶剂和封闭系统符合清洁生产的原则。快速处理、能源效率和可扩展性的综合优势使该方法成为工业规模生产高性能光催化复合材料的可行途径。微波辅助水热合成证明了工艺电气化，从传统的基于炉的热处理过渡到直接微波加热，从而降低了能耗和相关的二氧化碳排放。

{"title":"Microwave Electrification as a Process-Intensification Strategy for Calcination-Free, Scalable, and Sustainable Synthesis of Anatase-TiO2/α-Fe2O3 Photocatalysts","authors":"Praveen Kumar Lavudya,Sesha SuryaBindu Devarakonda,Dharani Kumar Chennamsetty,Nowduru Ravikiran,Venkata Satya Siva Srikanth Vadali,Rajanikanth Ammanabrolu","doi":"10.1021/acssuschemeng.5c12003","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c12003","url":null,"abstract":"While anatase-TiO2/α-Fe2O3 (ATAF) composites are promising visible-light photocatalysts, their conventional synthesis is hindered by prolonged processing and high-temperature calcination, which limits scalability and increases energy consumption. This work demonstrates a rapid, single-step microwave-hydrothermal strategy to fabricate phase-pure ATAF composites within 10 min, entirely without calcination. This method facilitates the heterogeneous nucleation of anatase-TiO2 onto α-Fe2O3 particles, creating an intimate interface. By optimizing the α-Fe2O3 content with uniform TiO2 decoration on it, an ATAF composite exhibiting superior charge separation, as evidenced by significant photoluminescence quenching, is prepared. This optimal interface engineering results in a remarkable 99.9% photocatalytic degradation of methylene blue under visible light, significantly outperforming the individual constituents. This energy-efficient approach potentially reduces synthesis energy consumption by one to 2 orders of magnitude compared to conventional calcination routes, while the use of aqueous solvents and a closed system aligns with the principles of clean production. The combined advantages of rapid processing, energy efficiency, and scalability position this method as a viable pathway for the industrial-scale production of high-performance photocatalytic composites. The microwave-assisted hydrothermal synthesis demonstrates process electrification by transitioning from conventional furnace-based thermal treatment to direct microwave heating, resulting in reduced energy consumption and associated CO2 emissions.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"7 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044928","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

Microwave Electrification as a Process-Intensification Strategy for Calcination-Free, Scalable, and Sustainable Synthesis of Anatase-TiO2/α-Fe2O3 Photocatalysts 微波电气化作为无煅烧、可扩展和可持续合成锐钛矿- tio2 /α-Fe2O3光催化剂的工艺强化策略

IF 8.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering

Pub Date : 2026-01-26 DOI: 10.1021/acssuschemeng.5c12003

Praveen Kumar Lavudya,Sesha SuryaBindu Devarakonda,Dharani Kumar Chennamsetty,Nowduru Ravikiran,Venkata Satya Siva Srikanth Vadali,Rajanikanth Ammanabrolu,Praveen Kumar Lavudya,Sesha SuryaBindu Devarakonda,Dharani Kumar Chennamsetty,Nowduru Ravikiran,Venkata Satya Siva Srikanth Vadali,Rajanikanth Ammanabrolu,Praveen Kumar Lavudya,Sesha SuryaBindu Devarakonda,Dharani Kumar Chennamsetty,Nowduru Ravikiran,Venkata Satya Siva Srikanth Vadali,Rajanikanth Ammanabrolu

While anatase-TiO2/α-Fe2O3 (ATAF) composites are promising visible-light photocatalysts, their conventional synthesis is hindered by prolonged processing and high-temperature calcination, which limits scalability and increases energy consumption. This work demonstrates a rapid, single-step microwave-hydrothermal strategy to fabricate phase-pure ATAF composites within 10 min, entirely without calcination. This method facilitates the heterogeneous nucleation of anatase-TiO2 onto α-Fe2O3 particles, creating an intimate interface. By optimizing the α-Fe2O3 content with uniform TiO2 decoration on it, an ATAF composite exhibiting superior charge separation, as evidenced by significant photoluminescence quenching, is prepared. This optimal interface engineering results in a remarkable 99.9% photocatalytic degradation of methylene blue under visible light, significantly outperforming the individual constituents. This energy-efficient approach potentially reduces synthesis energy consumption by one to 2 orders of magnitude compared to conventional calcination routes, while the use of aqueous solvents and a closed system aligns with the principles of clean production. The combined advantages of rapid processing, energy efficiency, and scalability position this method as a viable pathway for the industrial-scale production of high-performance photocatalytic composites. The microwave-assisted hydrothermal synthesis demonstrates process electrification by transitioning from conventional furnace-based thermal treatment to direct microwave heating, resulting in reduced energy consumption and associated CO2 emissions.

虽然锐钛矿- tio2 /α-Fe2O3 （ATAF）复合材料是很有前途的可见光催化剂，但其传统合成受到长时间加工和高温煅烧的阻碍，这限制了可扩展性并增加了能耗。这项工作展示了一种快速的单步微波热液策略，可以在10分钟内制造相纯ATAF复合材料，完全不需要煅烧。这种方法有利于锐钛矿- tio2在α-Fe2O3颗粒上的非均相成核，形成一个紧密的界面。通过对α-Fe2O3含量进行优化，并在α-Fe2O3表面均匀修饰，制备出具有良好电荷分离性能的ATAF复合材料，并具有明显的光致猝灭现象。这种优化的界面工程使得亚甲基蓝在可见光下的光催化降解率达到99.9%，显著优于单个组分。与传统的煅烧路线相比，这种节能方法有可能将合成能耗降低一到两个数量级，同时使用水性溶剂和封闭系统符合清洁生产的原则。快速处理、能源效率和可扩展性的综合优势使该方法成为工业规模生产高性能光催化复合材料的可行途径。微波辅助水热合成证明了工艺电气化，从传统的基于炉的热处理过渡到直接微波加热，从而降低了能耗和相关的二氧化碳排放。

{"title":"Microwave Electrification as a Process-Intensification Strategy for Calcination-Free, Scalable, and Sustainable Synthesis of Anatase-TiO2/α-Fe2O3 Photocatalysts","authors":"Praveen Kumar Lavudya,Sesha SuryaBindu Devarakonda,Dharani Kumar Chennamsetty,Nowduru Ravikiran,Venkata Satya Siva Srikanth Vadali,Rajanikanth Ammanabrolu,Praveen Kumar Lavudya,Sesha SuryaBindu Devarakonda,Dharani Kumar Chennamsetty,Nowduru Ravikiran,Venkata Satya Siva Srikanth Vadali,Rajanikanth Ammanabrolu,Praveen Kumar Lavudya,Sesha SuryaBindu Devarakonda,Dharani Kumar Chennamsetty,Nowduru Ravikiran,Venkata Satya Siva Srikanth Vadali,Rajanikanth Ammanabrolu","doi":"10.1021/acssuschemeng.5c12003","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c12003","url":null,"abstract":"While anatase-TiO2/α-Fe2O3 (ATAF) composites are promising visible-light photocatalysts, their conventional synthesis is hindered by prolonged processing and high-temperature calcination, which limits scalability and increases energy consumption. This work demonstrates a rapid, single-step microwave-hydrothermal strategy to fabricate phase-pure ATAF composites within 10 min, entirely without calcination. This method facilitates the heterogeneous nucleation of anatase-TiO2 onto α-Fe2O3 particles, creating an intimate interface. By optimizing the α-Fe2O3 content with uniform TiO2 decoration on it, an ATAF composite exhibiting superior charge separation, as evidenced by significant photoluminescence quenching, is prepared. This optimal interface engineering results in a remarkable 99.9% photocatalytic degradation of methylene blue under visible light, significantly outperforming the individual constituents. This energy-efficient approach potentially reduces synthesis energy consumption by one to 2 orders of magnitude compared to conventional calcination routes, while the use of aqueous solvents and a closed system aligns with the principles of clean production. The combined advantages of rapid processing, energy efficiency, and scalability position this method as a viable pathway for the industrial-scale production of high-performance photocatalytic composites. The microwave-assisted hydrothermal synthesis demonstrates process electrification by transitioning from conventional furnace-based thermal treatment to direct microwave heating, resulting in reduced energy consumption and associated CO2 emissions.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"1 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044926","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

Enhancing CO2 Hydrogenation to Methanol at Tunable Cu–ZnO Interfaces on Hydrotalcite-Derived Cu Nanocatalysts 在水滑石衍生的Cu纳米催化剂上，在可调Cu - zno界面上增强CO2加氢制甲醇

IF 8.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering

Pub Date : 2026-01-25 DOI: 10.1021/acssuschemeng.5c10863

Guoqing Cui, Yingjie Lou, Yiyang Hu, Mingxia Zhou, Yuming Li, Yajun Wang, Wei Wang, Jiong Li, Guiyuan Jiang, Chunming Xu

The hydrogenation of CO₂ to methanol serves as a practical approach extensively applied in achieving carbon cycling utilization and reducing carbon emissions. Nevertheless, the rational design of Cu-based catalysts with satisfactory catalytic performance and corresponding structure–activity relationship understanding still remains a challenging goal. Inspired by the characteristics of both hydrotalcite structures and active Cu species for CO₂ hydrogenation, a series of hydrotalcite-derived Cu nanocatalysts with highly dispersed Cu nanoclusters and tunable electronic and geometric structures are obtained via simply controlling structural topological transformation process temperature, verified by a comprehensive study including Bader charge analyses, TG-MS, HAADF-STEM, in situ CO–DRIFTS, and XAFS experiments. The optimized catalyst demonstrates an exceptional normalized CO₂ reaction rate of 30.6 mmol·g_cat^–1·h^–1 and a methanol selectivity of 92%, yielding an excellent methanol space-time yield (∼0.9 g·g_cat^–1·h^–1) and a stability of 100 h under mild conditions (220 °C, 3 MPa). This is approximately twice that of the control catalyst and ranks among the top outcomes reported so far for Cu-based systems. Operando FTIR, structure–activity relationship, and DFT studies elucidate that the active Cu species at the Cu–ZnO interface function as intrinsic active centers, accelerating the formation of key intermediates (HCOO* and H₃CO*), leading to a lower activation-energy barrier. Therefore, this work presents an effective strategy for fabricating Cu nanocatalysts featuring a precisely controllable Cu–ZnO interface via a facile LDH topological transformation, offering a promising application path in the large-scale synthesis of methanol from CO₂ hydrogenation.

二氧化碳加氢制甲醇是一种广泛应用于实现碳循环利用和减少碳排放的实用方法。然而，合理设计具有满意催化性能的铜基催化剂并理解相应的构效关系仍然是一个具有挑战性的目标。受水滑石结构和CO2加氢活性Cu物质特征的启发，通过简单控制结构拓扑转变过程温度，获得了一系列具有高度分散Cu纳米团簇和可调谐电子和几何结构的水滑石衍生Cu纳米催化剂，并通过Bader电荷分析、TG-MS、HAADF-STEM、原位CO-DRIFTS和XAFS实验等综合研究进行了验证。优化后的催化剂具有30.6 mmol·gcat-1·h - 1的标准化CO2反应速率和92%的甲醇选择性，在温和条件（220°C, 3 MPa）下，甲醇的时空产率为~ 0.9 g·gcat-1·h - 1，稳定性为100 h。这大约是对照催化剂的两倍，是迄今为止报道的cu基系统的最佳结果之一。FTIR、构效关系和DFT研究表明，Cu - zno界面处的活性Cu作为本构活性中心，加速了关键中间体（HCOO*和H3CO*）的形成，导致了较低的活化能垒。因此，本研究提出了一种有效的策略，通过简单的LDH拓扑变换制备具有精确可控Cu - zno界面的Cu纳米催化剂，为CO2加氢大规模合成甲醇提供了一条有前途的应用途径。

{"title":"Enhancing CO2 Hydrogenation to Methanol at Tunable Cu–ZnO Interfaces on Hydrotalcite-Derived Cu Nanocatalysts","authors":"Guoqing Cui, Yingjie Lou, Yiyang Hu, Mingxia Zhou, Yuming Li, Yajun Wang, Wei Wang, Jiong Li, Guiyuan Jiang, Chunming Xu","doi":"10.1021/acssuschemeng.5c10863","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c10863","url":null,"abstract":"The hydrogenation of CO2 to methanol serves as a practical approach extensively applied in achieving carbon cycling utilization and reducing carbon emissions. Nevertheless, the rational design of Cu-based catalysts with satisfactory catalytic performance and corresponding structure–activity relationship understanding still remains a challenging goal. Inspired by the characteristics of both hydrotalcite structures and active Cu species for CO2 hydrogenation, a series of hydrotalcite-derived Cu nanocatalysts with highly dispersed Cu nanoclusters and tunable electronic and geometric structures are obtained via simply controlling structural topological transformation process temperature, verified by a comprehensive study including Bader charge analyses, TG-MS, HAADF-STEM, in situ CO–DRIFTS, and XAFS experiments. The optimized catalyst demonstrates an exceptional normalized CO2 reaction rate of 30.6 mmol·gcat–1·h–1 and a methanol selectivity of 92%, yielding an excellent methanol space-time yield (∼0.9 g·gcat–1·h–1) and a stability of 100 h under mild conditions (220 °C, 3 MPa). This is approximately twice that of the control catalyst and ranks among the top outcomes reported so far for Cu-based systems. Operando FTIR, structure–activity relationship, and DFT studies elucidate that the active Cu species at the Cu–ZnO interface function as intrinsic active centers, accelerating the formation of key intermediates (HCOO* and H3CO*), leading to a lower activation-energy barrier. Therefore, this work presents an effective strategy for fabricating Cu nanocatalysts featuring a precisely controllable Cu–ZnO interface via a facile LDH topological transformation, offering a promising application path in the large-scale synthesis of methanol from CO2 hydrogenation.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"31 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044925","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

Dual-Function Reactive Extrusion of Lignocellulosic Fibers for High-Performance Biodegradable Nanocomposite Films 木质纤维素纤维双功能反应挤出制备高性能可生物降解纳米复合膜

IF 8.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering

Pub Date : 2026-01-25 DOI: 10.1021/acssuschemeng.5c11507

Kexin Zhou, Zihan Zhang, Junqi Gao, Bingqiang Pan, Kexia Jin, Yuxuan Xia, Da Zhang, Hongkun Wang, Yang Zhu, Wen-Jun Wang, Xuan Yang

The transition toward sustainable plastics calls for biodegradable polymers with enhanced performance and scalable processing routes. Plant-derived nanofibers are promising reinforcements, yet their adoption is hindered by energy-intensive isolation, incompatibility with hydrophobic matrices, and aggregation during drying. Here, we report a dual-function reactive extrusion strategy that combines nanofibrillation and surface modification in a single step. Lignocellulosic fibers are prefunctionalized with maleic anhydride to introduce carboxyl groups while retaining native lignin, and in-situ transesterification during melt compounding generates well-dispersed cellulose nanofibrils covalently bonded to PBAT. This integrated approach removes the need for costly nanocellulose isolation and drying while simultaneously ensuring compatibility and mechanical integrity through both chemical bonding and the hydrophobic contribution of lignin. The resulting composite films exhibit a 30% increase in stiffness while maintaining superior tensile strength and strain at failure, along with a 42% and 56% reduction in water vapor and oxygen permeability, respectively, compared to neat polymers. Additionally, the preserved lignin imparts over 90% antibacterial activity, enabling improved fruit preservation, while many film trials confirmed effective soil moisture retention and good biodegradability. Overall, this work establishes a scalable, industry-ready route to transform raw biomass into multifunctional nanofillers, providing a green pathway toward high-performance composite films for packaging and agricultural applications.

向可持续塑料的过渡需要具有增强性能和可扩展加工路线的可生物降解聚合物。植物源性纳米纤维是一种很有前途的增强材料，但它们的应用受到能量密集隔离、与疏水基质不相容以及干燥过程中的聚集等因素的阻碍。在这里，我们报告了一种双功能反应挤出策略，将纳米颤动和表面修饰结合在一个步骤中。木质纤维素纤维被马来酸酐预官能化以引入羧基，同时保留天然木质素，在熔融复合过程中原位酯交换生成分散良好的纤维素纳米原纤维，共价键与PBAT结合。这种综合方法消除了昂贵的纳米纤维素分离和干燥的需要，同时通过化学键和木质素的疏水性贡献确保相容性和机械完整性。与纯聚合物相比，复合膜的刚度增加了30%，同时在失效时保持了优异的抗拉强度和应变，水蒸气渗透率和氧气渗透率分别降低了42%和56%。此外，保存后的木质素具有超过90%的抗菌活性，从而改善了水果的保存，而许多薄膜试验证实了有效的土壤保湿性和良好的生物降解性。总的来说，这项工作建立了一个可扩展的、工业就绪的途径，将原料生物质转化为多功能纳米填料，为包装和农业应用的高性能复合薄膜提供了一条绿色途径。

{"title":"Dual-Function Reactive Extrusion of Lignocellulosic Fibers for High-Performance Biodegradable Nanocomposite Films","authors":"Kexin Zhou, Zihan Zhang, Junqi Gao, Bingqiang Pan, Kexia Jin, Yuxuan Xia, Da Zhang, Hongkun Wang, Yang Zhu, Wen-Jun Wang, Xuan Yang","doi":"10.1021/acssuschemeng.5c11507","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c11507","url":null,"abstract":"The transition toward sustainable plastics calls for biodegradable polymers with enhanced performance and scalable processing routes. Plant-derived nanofibers are promising reinforcements, yet their adoption is hindered by energy-intensive isolation, incompatibility with hydrophobic matrices, and aggregation during drying. Here, we report a dual-function reactive extrusion strategy that combines nanofibrillation and surface modification in a single step. Lignocellulosic fibers are prefunctionalized with maleic anhydride to introduce carboxyl groups while retaining native lignin, and in-situ transesterification during melt compounding generates well-dispersed cellulose nanofibrils covalently bonded to PBAT. This integrated approach removes the need for costly nanocellulose isolation and drying while simultaneously ensuring compatibility and mechanical integrity through both chemical bonding and the hydrophobic contribution of lignin. The resulting composite films exhibit a 30% increase in stiffness while maintaining superior tensile strength and strain at failure, along with a 42% and 56% reduction in water vapor and oxygen permeability, respectively, compared to neat polymers. Additionally, the preserved lignin imparts over 90% antibacterial activity, enabling improved fruit preservation, while many film trials confirmed effective soil moisture retention and good biodegradability. Overall, this work establishes a scalable, industry-ready route to transform raw biomass into multifunctional nanofillers, providing a green pathway toward high-performance composite films for packaging and agricultural applications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"44 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044871","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

Boosted Performance of Composite Cementitious Materials Derived from Incineration Fly Ash via Thermal Activation 热活化法提高焚烧飞灰复合胶凝材料性能

IF 7.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering

Pub Date : 2026-01-24 DOI: 10.1021/acssuschemeng.5c11668

Kailun Chen, , , Li Lin, , , Jinglin Li, , , Endian Hu, , , Jingwen Chang, , , Ke Liu, , and , Jianguo Jiang*,

Washing and thermal treatment are among the most promising technologies for managing municipal solid waste incineration fly ash (FA). However, the fate of residual ash after treatment remains uncertain and requires further investigation to achieve full resource utilization. In this study, the feasibility of using raw fly ash (RFA), washed fly ash (WFA), and thermally activated fly ash (TFA) as partial replacements for cement in composite cementitious materials was investigated. The macroscopic properties, strength development, environmental safety, and hydration mechanisms of FA-based composites were systematically examined. After the removal of hazardous substances, the physicochemical properties of WFA and TFA became closer to those of ordinary Portland cement (OPC). The mechanical performance of the composites followed the order TFA > WFA > RFA. At a 30% replacement level, the compressive strength of TFA reached 64.2 MPa, slightly higher than that of pure OPC and 103% greater than that of RFA. The corresponding carbon emission calibrated by strength is 29.5% lower than that of pure OPC, reaching 672.5 kgCO₂e/t. In terms of environmental performance, heavy-metal leaching from all FA-based composites met the relevant standards, and the chloride immobilization efficiency exceeded 90%. The crystalline phases of hydration products included ettringite (AFt), calcium silicate hydrate [C-(A)-S-H], and Friedel’s salt. During hydration, the formation of portlandite, precipitation of AFt, and deposition of C-(A)-S-H led to an interlaced microstructure in the TFA-derived composites, effectively refining the microstructure and thereby enhancing the macroscopic performance. These findings provide a reference pathway for the utilization of FA and contribute to the sustainable management of FA.

洗涤和热处理是处理城市固体垃圾焚烧飞灰最有前途的技术。然而，处理后的残灰的命运仍然不确定，需要进一步研究，以实现充分的资源利用。在本研究中，研究了在复合胶凝材料中使用生粉煤灰（RFA）、水洗粉煤灰（WFA）和热活化粉煤灰（TFA）部分替代水泥的可行性。系统地研究了fa基复合材料的宏观性能、强度发展、环境安全性和水化机理。在去除有害物质后，WFA和TFA的物理化学性能更接近于普通硅酸盐水泥（OPC）。复合材料的力学性能表现为TFA >； WFA >； RFA。在30%替代水平下，TFA的抗压强度达到64.2 MPa，略高于纯OPC，比RFA高103%。与纯OPC相比，强度标定的碳排放量降低了29.5%，达到672.5 kgCO2e/t。在环保性能方面，fa基复合材料重金属浸出均达到相关标准，氯离子固定化效率超过90%。水化产物的晶相包括钙矾石（AFt）、水合硅酸钙[C-(A)- s - h]和弗里德尔盐。水化过程中，硅酸盐的形成、AFt的沉淀和C-(A)- s - h的沉积导致tfa衍生复合材料的微观结构呈交错状，有效地细化了微观结构，从而提高了宏观性能。研究结果为农用植物资源的利用提供了参考途径，有助于农用植物资源的可持续管理。

{"title":"Boosted Performance of Composite Cementitious Materials Derived from Incineration Fly Ash via Thermal Activation","authors":"Kailun Chen, , , Li Lin, , , Jinglin Li, , , Endian Hu, , , Jingwen Chang, , , Ke Liu, , and , Jianguo Jiang*, ","doi":"10.1021/acssuschemeng.5c11668","DOIUrl":"10.1021/acssuschemeng.5c11668","url":null,"abstract":"Washing and thermal treatment are among the most promising technologies for managing municipal solid waste incineration fly ash (FA). However, the fate of residual ash after treatment remains uncertain and requires further investigation to achieve full resource utilization. In this study, the feasibility of using raw fly ash (RFA), washed fly ash (WFA), and thermally activated fly ash (TFA) as partial replacements for cement in composite cementitious materials was investigated. The macroscopic properties, strength development, environmental safety, and hydration mechanisms of FA-based composites were systematically examined. After the removal of hazardous substances, the physicochemical properties of WFA and TFA became closer to those of ordinary Portland cement (OPC). The mechanical performance of the composites followed the order TFA > WFA > RFA. At a 30% replacement level, the compressive strength of TFA reached 64.2 MPa, slightly higher than that of pure OPC and 103% greater than that of RFA. The corresponding carbon emission calibrated by strength is 29.5% lower than that of pure OPC, reaching 672.5 kgCO2e/t. In terms of environmental performance, heavy-metal leaching from all FA-based composites met the relevant standards, and the chloride immobilization efficiency exceeded 90%. The crystalline phases of hydration products included ettringite (AFt), calcium silicate hydrate [C-(A)-S-H], and Friedel’s salt. During hydration, the formation of portlandite, precipitation of AFt, and deposition of C-(A)-S-H led to an interlaced microstructure in the TFA-derived composites, effectively refining the microstructure and thereby enhancing the macroscopic performance. These findings provide a reference pathway for the utilization of FA and contribute to the sustainable management of FA.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"14 5","pages":"2556–2569"},"PeriodicalIF":7.3,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034169","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