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Solvent effects on recyclability of Amberlyst-15 in catalyzing high-concentration fructose to 5-hydroxymethylfurfural 溶剂对Amberlyst-15催化高浓度果糖制5-羟甲基糠醛可回收性的影响
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-14 DOI: 10.1016/j.jece.2026.121268
Yexin Hu, Qingju Yan, Jiangbo Ran, Liangzhang He, Weiyang Chen, Yimin Shan
Achieving large-scale production of biomass-derived 5-hydroxymethylfurfural (HMF) hinges on the high-concentration substrate and an effective recyclability of catalysts. Amberlyst-15 (A15) is a commercial sulfonated ion-exchange resin commonly used to catalyze the fructose-to-HMF dehydration. However, comparative studies on its recyclability during the conversion of high-concentration fructose in different solvents remain limited. Herein, we investigate the relationship between the recyclability of A15 and reaction solvents in dehydration of high-concentration fructose (20.0 wt.%) by recyclable experiments of A15 in H2O, THF, 1,4-dioxane, DMSO, and DMSO-H2O co-solvents with different water content at 140 ℃, wherein the worst recyclability is observed in THF and 1,4-dioxane. By comparing the structure of the A15 catalyst before and after the reaction and following solvothermal treatment, it was found that the primary factor hindering catalyst recyclability is the carbon deposit composed of humins on the surface of A15. Among these, the most severe humins formed through etherification-dehydration-condensation reactions and degradative condensation reactions of fructose and/or HMF are observed in THF and 1,4-dioxane. Furthermore, as the water content in the DMSO-H2O co-solvent increases, the formation of humins I via etherification-dehydration-condensation path intensifies, whereas the formation of humins II via degradative condensation path would be diminishes. Overall, water content exerts negligible influence on total production of humins and the recyclability of the A15 catalyst. This work highlights the relationship between catalyst recyclability and solvent-controlled humin formation mechanisms, providing critical insights for developing sustainable solvent systems suitable for HMF biorefineries.
实现生物质衍生5-羟甲基糠醛(HMF)的大规模生产取决于高浓度的底物和催化剂的有效可回收性。Amberlyst-15 (A15)是一种商业磺化离子交换树脂,通常用于催化果糖脱水制hmf。然而,对高浓度果糖在不同溶剂转化过程中其可回收性的比较研究仍然有限。本研究通过对A15在水、四氢呋喃、1,4-二恶烷、DMSO和DMSO-H2O等不同含水量的共溶剂中在140℃条件下的可回收性实验,考察了A15在高浓度果糖(20.0 wt.%)脱水过程中的可回收性与反应溶剂的关系,其中四氢呋喃和1,4-二恶烷的可回收性最差。通过比较反应前后和溶剂热处理后A15催化剂的结构,发现阻碍催化剂可回收性的主要因素是A15表面由人因组成的积碳。其中,通过醚化-脱水-缩合反应和果糖和/或HMF的降解缩合反应形成的最严重的人因是在THF和1,4-二恶烷中观察到的。此外,随着DMSO-H2O共溶剂中含水量的增加,通过醚化-脱水-缩合途径生成人蛋白I的能力增强,而通过降解缩合途径生成人蛋白II的能力减弱。总体而言,水含量对人类素总产量和A15催化剂可回收性的影响可以忽略不计。这项工作强调了催化剂可回收性和溶剂控制的人类形成机制之间的关系,为开发适用于HMF生物炼制的可持续溶剂系统提供了重要见解。
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引用次数: 0
Effects of polyethylene microplastics and 6PPD co-contamination on black soil 聚乙烯微塑料与6PPD共污染对黑土的影响
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-14 DOI: 10.1016/j.jece.2026.121245
Hengle Niu , Yang Yang , Yufeng Bai , Yong Yu
The widespread detection of microplastics (MPs) in various ecosystems has been widely reported. 6PPD (N-(1,3-dimethylbutyl)-N′-phenyl-p-phenylenediamine) is a synthetic antioxidant, which can be adsorbed by MPs and lead to combined contaminants. The impact of both individual and co-contamination with PE-MPs and 6PPD on soil was evaluated in this study, focusing on its physicochemical properties and microbial communities. The results indicated that soil ammonium nitrogen (NH4+-N) content was significantly increased by 26.88 % in the T7 group (500 mg/kg PE-MPs + 0.1 mg/kg 6PPD) compared to the CK. The structure of the soil microbial community was affected, and the Shannon index was significantly reduced by 11.38 % under high-concentration combined pollution. A concentration-dependent effect of PE-MPs and 6PPD on bacterial community connections was observed in microbial community networks, along with an increase in the complexity of microbial community networks caused by high-concentration combined contamination. Redundancy analysis and mantel test indicated that soil pH, available phosphorus (AP), NH4+-N, and nitrate nitrogen (NO3--N) were the key environmental factors in influencing the soil microbial community. Kyoto Encyclopedia of Genes and Genomes (KEGG) pathway analysis indicated that Metabolism was the predominant functional category, accounting for approximately 70.3 % of the functional annotations. This study reveals the implications of PE-MPs and 6PPD co-contamination for environmental risks and soil health.
微塑料(MPs)在各种生态系统中的广泛检测已被广泛报道。6PPD (N-(1,3-二甲基丁基)-N ' -苯基-对苯二胺)是一种合成抗氧化剂,可被MPs吸附并导致复合污染物。本研究评估了PE-MPs和6PPD单独污染和共同污染对土壤的影响,重点是其理化性质和微生物群落。结果表明:与对照相比,T7处理(500 mg/kg PE-MPs + 0.1 mg/kg 6PPD)显著提高了土壤铵态氮(NH4+-N)含量26.88 %;高浓度复合污染影响了土壤微生物群落结构,Shannon指数显著降低11.38 %。在微生物群落网络中观察到PE-MPs和6PPD对细菌群落连接的浓度依赖效应,以及高浓度复合污染引起的微生物群落网络复杂性的增加。冗余分析和mantel试验表明,土壤pH、速效磷(AP)、NH4+-N和硝态氮(NO3—N)是影响土壤微生物群落的关键环境因子。京都基因与基因组百科(KEGG)通路分析表明,代谢是主要的功能类别,约占70.3 %的功能注释。本研究揭示了PE-MPs和6PPD共污染对环境风险和土壤健康的影响。
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引用次数: 0
Tracing antibiotic fate in Chinese sea bass aquaculture: Implications for food safety and sustainability 追踪中国黑鲈养殖中的抗生素命运:对食品安全和可持续性的影响
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-14 DOI: 10.1016/j.jece.2026.121237
Haochang Su , Nanzhen Yi , Xiaoyang Zhang , Xiaojuan Hu , Wujie Xu , Yu Xu , Guoliang Wen , Yucheng Cao
Antibiotics are emerging contaminants. Systematic studies on the source tracing, dissemination and its key drivers of antibiotics in aquaculture, as well as their environmental fate, remain scarce. This study investigated the distribution, accumulation, and environmental fate of antibiotics within sea bass aquaculture systems in China's Sea Bass Capital, with a emphasis on the influence of antibiotic physicochemical properties on their behavior in water, sediment, and biota. Results showed that the molecular weight and octanol-water partition coefficient (Kow) of antibiotics significantly influenced their bioaccumulation in aquaculture organisms, underscoring the pivotal role of these properties in driving the distribution of antibiotics in aquatic environments. Furthermore, solubility and Kow of antibiotics were identified as critical factors affecting their partitioning between aqueous and sediment phases. Suspended solids were identified as a key driver for the spread and distribution of antibiotics within the system. Quinolone antibiotics, due to their prevalence and potential environmental impact, have been identified as key indicator antibiotics for priority management and control. Over half of the antibiotic remained in the sediment, with 30 % naturally degraded. This study elucidates the environmental trajectory of antibiotics, shedding light on their potential threats to aquatic ecosystems and food safety. It underscores the pivotal role of prudent waste management practices for antibiotics in aquaculture. Our findings can guide the formulation of specific mitigation strategies and enrich the ongoing dialogue on environmental sustainability and food safety.
抗生素是新兴的污染物。关于水产养殖中抗生素的来源追踪、传播及其主要驱动因素及其环境命运的系统研究仍然很少。本研究调查了中国黑鲈之都养殖系统中抗生素的分布、积累和环境命运,重点研究了抗生素理化性质对其在水、沉积物和生物群中的行为的影响。结果表明,抗生素的分子量和辛醇-水分配系数(辛醇-水分配系数,Kow)显著影响其在水产养殖生物体内的生物蓄积,这些特性在驱动抗生素在水生环境中的分布中起着关键作用。此外,抗生素的溶解度和溶解度是影响其在水相和沉积物相之间分配的关键因素。悬浮物被确定为系统内抗生素传播和分布的关键驱动因素。喹诺酮类抗生素由于其普遍存在和潜在的环境影响,已被确定为重点管理和控制的关键指标抗生素。超过一半的抗生素留在沉积物中,30% %自然降解。本研究阐明了抗生素的环境轨迹,揭示了抗生素对水生生态系统和食品安全的潜在威胁。它强调了水产养殖中谨慎的抗生素废物管理做法的关键作用。我们的研究结果可以指导制定具体的缓解战略,并丰富正在进行的关于环境可持续性和食品安全的对话。
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引用次数: 0
Monolithic adsorbent with low pressure drop and high cycling stability enabled by an anchor effect for direct air CO2 capture 整体吸附剂具有低压降和高循环稳定性,通过锚定效应实现直接空气CO2捕获
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-14 DOI: 10.1016/j.jece.2026.121233
Peng Yuan, FeiFan Huang, PeiJun Li, HuiXian Tian, YuChen Zhou, Tao Li
The continuous rise in atmospheric CO2 is a major driver of global warming, creating the urgent need for negative emission technologies. Direct air capture (DAC) based on solid amine adsorbents has attracted increasing attention due to their balanced performance in capacity, cost, and scalable fabrication. However, DAC operation typically requires high gas flow rates, making low pressure drop and strong support-active phase binding critical to limiting fan energy consumption and ensuring long-term durability. To address this challenge, a four-channel micro-monolithic adsorbent was developed using an alumina ceramic support, polyethyleneimine (PEI) as the active phase, and 3-aminopropyltriethoxysilane (APS) as a coupling agent. The results indicate that APS effectively enhances PEI dispersion and anchoring, enabling a CO2 adsorption capacity of 0.61 mmol/g, stable performance over 15 adsorption-desorption cycles, and robust tolerance to humidity (0–100 % RH) and temperatures (30–50℃). In addition, the continuous channel architecture results in a low pressure drop of only 4.9–9.8 Pa/cm at gas velocities of 0.53–1.06 m/s, corresponding to a 75.5–83.8 % reduction compared with conventional monoliths. Overall, this work provides a promising micro-monolithic adsorbent platform for scalable and energy-efficient DAC deployment.
大气中二氧化碳的持续上升是全球变暖的主要驱动因素,因此迫切需要负排放技术。基于固体胺吸附剂的直接空气捕获(DAC)由于其在容量、成本和可扩展制造方面的平衡性能而受到越来越多的关注。然而,DAC操作通常需要高气体流速,因此低压降和强支撑有源相结合对于限制风扇能耗和确保长期耐用性至关重要。为了解决这一问题,研究人员开发了一种四通道微单片吸附剂,该吸附剂采用氧化铝陶瓷载体,聚乙烯亚胺(PEI)作为活性相,3-氨基丙基三乙氧基硅烷(APS)作为偶联剂。结果表明,APS有效地增强了PEI的分散和锚定,使CO2吸附量达到0.61 mmol/g,在15个吸附-解吸循环中性能稳定,对湿度(0-100 % RH)和温度(30-50℃)具有较强的耐受性。此外,连续通道结构在气体速度为0.53-1.06 m/s时的低压降仅为4.9-9.8 Pa/cm,与传统单体相比降低了75.5-83.8 %。总的来说,这项工作为可扩展和节能的DAC部署提供了一个有前途的微单片吸附剂平台。
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引用次数: 0
Study on the mechanism by which CuO nanofluids regulate the interfacial wettability of coal 氧化铜纳米流体调节煤界面润湿性的机理研究
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-14 DOI: 10.1016/j.jece.2026.121224
Lei Fang , Jiangshi Zhang , Pengcheng Liu , Linquan Tong , Yunfei Liang , Zhongbin Zhang , Hongfu Jia , Qi Zhang , Jie Jiang
To develop an efficient, stable, and environmentally friendly wetting modification system for coal interfaces, this study investigates the wetting modification of intrinsically hydrophobic coal surfaces using CuO nanofluids with different particle sizes. By com-bining macroscopic wetting experiments with X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), zeta potential measurements, and molecular dy-namics simulations, an integrated and environmentally friendly nanofluid-based wetting modification framework is established to elucidate the regulation mechanisms at the coal–water interface. The results demonstrate that CuO nanoparticles can adsorb onto coal surfaces and form a stable hydrophilic layer, thereby significantly reducing interfa-cial energy and reconstructing adsorption structures as well as interfacial water behavior. CuO nanofluids markedly decrease the equilibrium contact angle of coal surfaces, with smaller particle sizes and higher concentrations being more favorable for enhancing in-terfacial spreading and adsorption. Owing to stronger interfacial energy regulation and more effective pore-scale wetting, smaller CuO nanoparticles exhibit higher interfacial activity and larger wetted areas. Stability analyses indicate that nanoparticles with small-er sizes possess superior dispersion stability due to enhanced Brownian motion, whereas the stability of the system gradually decreases with increasing particle size and concen-tration. CuO adsorption increases the negative surface charge and polarity of coal, thereby promoting the adsorption of polar molecules, with both adsorption capacity and surface coverage showing strong particle-size dependence. Molecular dynamics simula-tions further reveal that the introduction of CuO thickens the interfacial water layer, re-duces water diffusivity, promotes the transformation of free water into adsorbed water, and strengthens interfacial hydrogen-bonding and coordination structures. Importantly, water adsorption on CuO surfaces is not dominated by van der Waals interactions but is primarily governed by electrostatic interactions.
为了开发一种高效、稳定、环保的煤界面润湿改性体系,本研究利用不同粒径的氧化铜纳米流体对煤表面进行润湿改性。通过宏观润湿实验、x射线光电子能谱(XPS)、扫描电镜(SEM)、zeta电位测量和分子动力学模拟相结合,建立了一个完整的环境友好型纳米流体润湿改性框架,阐明了煤水界面的调控机制。结果表明,纳米CuO颗粒可以吸附在煤表面,形成稳定的亲水层,从而显著降低界面能,重构吸附结构和界面水行为。CuO纳米流体显著降低了煤表面的平衡接触角,粒径越小、浓度越高越有利于促进界面扩展和吸附。由于更强的界面能调节和更有效的孔隙尺度润湿,较小的CuO纳米颗粒具有更高的界面活性和更大的润湿面积。稳定性分析表明,粒径较小的纳米颗粒由于增强的布朗运动而具有较好的分散稳定性,而随着粒径和浓度的增加,系统的稳定性逐渐降低。CuO吸附增加了煤的表面负电荷和极性,从而促进了极性分子的吸附,吸附容量和表面覆盖率都表现出很强的粒径依赖性。分子动力学模拟进一步揭示了CuO的引入使界面水层增厚,降低了水的扩散系数,促进了自由水向吸附水的转变,增强了界面氢键和配位结构。重要的是,水在CuO表面的吸附不受范德华相互作用的支配,而主要受静电相互作用的支配。
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引用次数: 0
Seasonal and process-dependent microbial dynamics drive performance variations in full-scale AAO and modified UNITANK sewage treatment systems 季节性和过程相关的微生物动力学驱动全尺寸AAO和改进UNITANK污水处理系统的性能变化
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-14 DOI: 10.1016/j.jece.2026.121225
Xiaodan Gu , Feng Wang , Wei Wang , Chuangchuang Gao , Yongwei Ding
Urban sewage treatment plants (STPs) are critical for pollutant control, with microbial communities governing activated sludge (AS) treatment efficiency. This study explored seasonal and process impacts on microbial dynamics and pollutant removal in two full-scale STPs over one year: FX (parallel AAO and modified UNITANK) and LJ (only modified UNITANK). All processes showed 8.73–31.04 % higher chemical oxygen demand (COD) and 4.91–27.90 % higher total phosphorus (TP) removal in summer than winter. NH4+ -N (≥95 %) and TN (≥77.90 %) removal remained seasonally stable. FX AAO outperformed in COD (winter: 83.92 ± 13.58 %; summer: 92.65 ± 4.44 %) and TN removal (winter: 81.34 ± 6.44 %; summer: 83.32 ± 4.16 %), while LJ modified UNITANK excelled in TP removal (winter: 89.99 ± 7.38 %; summer: 94.90 ± 5.15 %). Summer enhanced microbial diversity, with FX modified UNITANK showing the highest diversity. At the phylum level, Proteobacteria, Actinobacteriota, and Bacteroidota dominated. At the genus level, Saccharofermentans was stable, nitrifiers and denitrifiers were low but consistent, polyphosphate-accumulating organisms (PAOs) were scarce (0.02–0.28 %), and glycogen-accumulating organisms (GAOs) were more abundant in summer (3.11–6.82 %) than winter (0.58–1.23 %), with the highest summer GAO levels observed in FX AAO. Saprospiraceae (dominant denitrifying PAO) favored FX AAO’s stable anoxic niches in winter (8.04–8.31 %) and FX modified UNITANK’s intermittent anoxic phases in summer (3.37–4.15 %). Mantel tests identified water temperature, sludge retention time, dissolved oxygen, hydraulic retention time, and influent COD loading as key drivers of microbial structure. This study advances understanding of AS microbial ecology regulation by seasons and processes, providing a basis for optimizing full-scale STP performance.
城市污水处理厂(STPs)是污染物控制的关键,微生物群落控制活性污泥(AS)的处理效率。本研究探讨了季节和工艺对两个大型污水处理厂一年内微生物动力学和污染物去除的影响:FX(平行AAO和改良UNITANK)和LJ(仅改良UNITANK)。夏季各处理的化学需氧量(COD)比冬季高8.73 ~ 31.04 %,总磷(TP)去除率比冬季高4.91 ~ 27.90 %。NH4+ -N(≥95 %)和TN(≥77.90 %)去除率保持季节稳定。外汇的氧化铝优于鳕鱼(冬天:83.92 ±13.58  %;夏天:92.65 ±4.44  %)和TN去除(冬天:81.34 ±6.44  %;夏天:83.32 ±4.16  %),而LJ修改UNITANK擅长TP去除(冬天:89.99 ±7.38  %;夏天:94.90 ±5.15  %)。夏季微生物多样性增强,FX修饰的UNITANK多样性最高。在门水平上,变形菌门、放线菌门和拟杆菌门占主导地位。在属水平上,糖化菌稳定,硝化菌和反硝化菌数量少但一致,聚磷菌(PAOs)较少(0.02 ~ 0.28 %),糖原积累菌(GAOs)在夏季较多(3.11 ~ 6.82 %),冬季较少(0.58 ~ 1.23 %),夏季最高的是FX AAO。sprospiraceae(优势反硝化PAO)在冬季有利于FX AAO的稳定缺氧生态位(8.04-8.31 %),FX修饰了UNITANK在夏季的间歇缺氧期(3.37-4.15 %)。Mantel试验确定水温、污泥滞留时间、溶解氧、水力滞留时间和进水COD负荷是微生物结构的关键驱动因素。该研究促进了对AS微生物生态随季节和过程的调控的认识,为全面优化STP性能提供了基础。
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引用次数: 0
Co-addition of alkali lignin and microbial agents drives humic substances assembly by regulating precursor conversion and microbial metabolism in composting 碱木质素和微生物剂的共同添加通过调节堆肥前体转化和微生物代谢来驱动腐殖质物质的组装
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-14 DOI: 10.1016/j.jece.2026.121188
Hongquan Xiang , Shiyuan Niu , De Ding , Binfeng Lin , Yu Zhang , Yongwei Zhu , Shiqiang Li , Ziyang Zhao , Jianbin Li , Zhi Huang
Sulfitation filter mud, an organic solid waste byproduct of sugar manufacturing, requires effective resource recovery strategies. Traditional composting methods for this material are characterized by low humification efficiency and prolonged processing times. This study investigated the effects of the independent and combined addition of alkali lignin (AL) and microbial agents (BL) on the humification process during sulfitation filter mud composting. The results showed that the combined addition (BA) resulted in the highest organic matter degradation rate (17.71 %) and the highest seed germination rate (141.18 %). Furthermore, the BA treatment significantly facilitated the transformation of fulvic acid (FA) into humic acid (HA). Compared to the control (CK), HA content and the HA/FA ratio increased by 42.5 % and 27.5 %, respectively. Three-dimensional excitation-emission matrix (3D-EEM) spectral analysis indicated that the addition of BA promoted the conversion of protein-like substances into humic substances. Metagenomic analysis showed that BA enhanced the relative abundance of Actinomycetota and Pseudomonas and strengthened the interactions among microorganisms, humic substances, and humic precursors. This research provides new insights into accelerating the humification process during composting and enhancing the humic substances content in the resulting compost.
硫酸过滤泥是制糖过程中产生的一种有机固体废弃物,需要有效的资源回收策略。这种材料的传统堆肥方法具有腐殖质化效率低、处理时间长等特点。研究了碱木质素(AL)和微生物剂(BL)单独和联合添加对硫化过滤泥堆肥腐殖质化过程的影响。结果表明,复合添加(BA)的有机物降解率最高(17.71 %),种子发芽率最高(141.18 %)。此外,BA处理显著促进了黄腐酸(FA)向腐植酸(HA)的转化。与对照(CK)相比,HA含量和HA/FA比分别提高了42.5 %和27.5% %。三维激发-发射矩阵(3D-EEM)光谱分析表明,BA的加入促进了类蛋白物质向腐殖质物质的转化。宏基因组分析表明,BA增加了放线菌门和假单胞菌的相对丰度,加强了微生物与腐殖质和腐殖质前体的相互作用。本研究为加速堆肥腐殖质化过程和提高堆肥中腐殖质含量提供了新的见解。
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引用次数: 0
Carbon nanotubes–supported photocatalysts for the reduction of CO2 into high-value products: A concise review 碳纳米管负载光催化剂将二氧化碳还原为高价值产品:简要综述
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-14 DOI: 10.1016/j.jece.2026.121232
Nady Fathy , Zhang Xin , Xingwang Zhu
Photocatalytic conversion of carbon dioxide (CO2) into high value-added fuels and chemicals represents a promising and sustainable approach to mitigating greenhouse gas emissions while enabling solar fuel production. Carbon nanotubes (CNTs) have gained considerable attention as catalyst supports for CO2 photoreduction due to their exceptional electrical conductivity, large specific surface area, tunable surface chemistry, and strong ability to enhance light absorption and charge separation. This review presents a comprehensive and up-to-date overview of CNTs-supported photocatalysts for CO2 conversion, encompassing fundamental reaction pathways, the photocatalytically relevant properties of CNTs, and diverse synthesis strategies for CNTs–photocatalyst composites incorporating metals, metal oxides, and cocatalysts. A comparative summary table highlights numerous CNTs-based systems and their performance metrics. Finally, the review outlines key challenges, strategies for improving reproducibility, and future directions for scaling up CO2 photoconversion technologies.
光催化将二氧化碳(CO2)转化为高附加值的燃料和化学品是一种有前途的可持续方法,可以在减少温室气体排放的同时实现太阳能燃料的生产。碳纳米管(Carbon nanotubes, CNTs)由于其优异的导电性、大的比表面积、可调的表面化学性质以及增强光吸收和电荷分离的能力,作为CO2光还原催化剂载体受到了广泛的关注。本文综述了碳纳米管支持的二氧化碳转化光催化剂的最新研究进展,包括基本的反应途径、碳纳米管的光催化相关性质,以及碳纳米管-光催化剂复合材料(包括金属、金属氧化物和助催化剂)的合成策略。比较汇总表突出了许多基于碳纳米管的系统及其性能指标。最后,综述概述了关键挑战,提高可重复性的策略,以及扩大二氧化碳光转换技术的未来方向。
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引用次数: 0
Selective catalytic conversion of polyphenylene oxide waste into benzene and toluene for hydrogen storage via zeolite-controlled hydro-pyrolysis 沸石控制加氢热解将聚苯乙烯氧化废选择性催化转化为苯和甲苯储氢
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-14 DOI: 10.1016/j.jece.2026.121267
Bingqing Shi , Dongxian Li , Xi Lin , Shule Wang , Xianzhi Meng , Yanghao Jin , Jia Wang , Jianchun Jiang
The selective conversion of plastic waste into benzene and toluene (BT) offers a promising route for producing Liquid Organic Hydrogen Carriers (LOHCs). This approach supports both carbon recycling and long-distance hydrogen storage. However, conventional catalytic pathways suffer from limited selectivity and frequent reliance on noble-metal catalysts for hydrogen-assisted deoxygenation. Here, we present a metal-free catalytic strategy that transforms Polyphenylene Oxide (PPO), an engineering thermoplastic with an aromatic-rich backbone, into high-purity BT aromatics under 0.2 MPa hydrogen pressure. A range of zeolite catalysts with varied topologies and acidities (HZSM-5, SAPO-34, USY, HSSZ-13, HZSM-11) were systematically evaluated. HZSM-5 exhibited the highest BT selectivity (>88 %) with minimal polyaromatic byproducts. Mechanistic studies reveal that moderate Brønsted acidity and medium-pore confinement in HZSM-5 play key roles. These features facilitate efficient ether bond cleavage and selective hydrogen-assisted Direct Deoxygenation (DDO) of methylated phenolic intermediates. Structure–activity correlations highlight the importance of pore architecture and acidity. Proper design promotes monoaromatic formation while suppressing side reactions. This work establishes a scalable, metal-free platform for converting oxygenated plastic waste into LOHC molecules. The strategy offers integrated solutions for plastic upcycling and clean hydrogen energy systems.
塑料废弃物选择性转化为苯和甲苯(BT)为生产液态有机氢载体(lohc)提供了一条很有前途的途径。这种方法既支持碳回收,也支持远距离储氢。然而,传统的催化途径选择性有限,并且经常依赖于贵金属催化剂进行氢辅助脱氧。在这里,我们提出了一种无金属催化策略,在0.2 MPa的氢压力下,将聚苯二烯氧化物(PPO)转化为高纯度的BT芳烃,PPO是一种具有丰富芳烃骨架的工程热塑性塑料。对具有不同拓扑结构和不同酸度的沸石催化剂(HZSM-5、SAPO-34、USY、HSSZ-13、HZSM-11)进行了系统评价。HZSM-5表现出最高的BT选择性(>88 %)和最少的多芳副产物。机理研究表明,HZSM-5的中等Brønsted酸性和中等孔隙约束是关键作用。这些特征有助于有效的醚键裂解和选择性氢辅助直接脱氧(DDO)甲基化酚中间体。结构-活性对比强调了孔隙结构和酸度的重要性。适当的设计促进单芳香族的形成,同时抑制副反应。这项工作建立了一个可扩展的无金属平台,用于将含氧塑料废物转化为LOHC分子。该战略为塑料升级回收和清洁氢能源系统提供了综合解决方案。
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引用次数: 0
Simultaneous removal of dolomite and feldspar from apatite by reverse flotation: Special selectivity of mixed anionic/cationic collectors 反浮选法同时从磷灰石中去除白云石和长石:阴离子/阳离子混合捕收剂的特殊选择性
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-14 DOI: 10.1016/j.jece.2026.121247
Donglang Li , Yangge Zhu , Dashi Lei , Xiaoliang Zhang , Xiyu Gao , Xiaoxing Hu , Songqing Li
Reverse flotation of gangue minerals, such as dolomite and feldspar, from apatite is a common process in phosphate ore beneficiation. However, conventional multi-stage flotation processes are often inefficient due to their complexity and high reagent consumption. This study proposes a simplified one-step flotation process utilizing a mixed anionic/cationic collector to simultaneously remove dolomite and feldspar from apatite. Flotation tests using artificial mixed minerals showed that the simultaneous removal rates of dolomite and feldspar exceeded 75 %. Zeta potential measurements, adsorption amount measurements, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), time-of-flight secondary ion mass spectrometry (ToF-SIMS), and molecular dynamics (MD) simulations were employed to elucidate the synergistic mechanism between the anionic and cationic collectors during flotation. Specifically, during flotation, sodium linolenic acid (SLA) and dioctyldimethyl ammonium chloride (DAC) individually acted as the primary collectors responsible for modifying the floatability of dolomite and feldspar, respectively. When combined into a mixed collector system, they not only maintained high removal efficiency for both minerals but also exhibited a synergistic effect that enhanced collector adsorption. Moreover, the mixed collectors formed unique molecular arrangements at the gas–liquid interface, improving foam fluidity and partially eliminating the problem of amine flotation foam over-stability. This study provides novel insights into phosphate ore separation and offers valuable information for the interfacial behavior of anionic/cationic collector systems.
从磷灰石中反浮选白云石、长石等脉石矿物是磷矿选矿中常见的工艺。然而,传统的多级浮选工艺由于其复杂性和高药剂消耗而往往效率低下。本研究提出了一种简化的一步浮选工艺,利用阴离子/阳离子混合捕收剂同时从磷灰石中去除白云石和长石。人工混合矿物浮选试验表明,白云石和长石的同时去除率超过75% %。采用Zeta电位测量、吸附量测量、傅里叶变换红外光谱(FTIR)、x射线光电子能谱(XPS)、飞行时间二次离子质谱(ToF-SIMS)和分子动力学(MD)模拟等方法,探讨了阴离子捕收剂和阳离子捕收剂在浮选过程中的协同作用机理。具体而言,在浮选过程中,亚麻酸钠(SLA)和二辛基二甲基氯化铵(DAC)分别作为主要捕收剂,负责改变白云石和长石的可浮性。当组合成混合捕收剂系统时,它们不仅保持了对两种矿物的高去除效率,而且表现出协同效应,增强了捕收剂的吸附。此外,混合捕收剂在气液界面形成独特的分子排列,提高了泡沫的流动性,部分消除了胺浮选泡沫的过稳定问题。该研究为磷矿分离提供了新的见解,并为阴离子/阳离子捕收剂系统的界面行为提供了有价值的信息。
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Journal of Environmental Chemical Engineering
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