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Sludge-derived hydrochar enhances anaerobic digestion of sludge with tetracycline: Focusing on synergistic mechanism and microbial response 污泥衍生碳氢化合物增强污泥与四环素厌氧消化:聚焦协同机制和微生物响应
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-15 DOI: 10.1016/j.jece.2026.121256
Jiaojiao Shi , Guoqing Li , Saiyu Yuan , Zhouyang Lian , Shengwei Wang , Huiwen Zhang
Anaerobic digestion is an effective strategy for the degradation of organic matter and recovery of high value-added products. While the inhibitory effect of antibiotics such as tetracycline (TC) on anaerobic digestion is known, and though biochar-based carriers have been explored to mitigate such inhibition, the potential of hydrocha to simultaneously remove antibiotics and enhance microbial activity remains unclear. In this study, sludge-derived hydrothermal carbon prepared with rice husk (SHC-IV) was applied as a bio-carrier to enhance the anaerobic digestion performance of tetracycline(TC)-contaminated sludge. Results showed that moderate TC addition (TC100) improved methane production, with a maximum cumulative yield of 44.97 mL/g·VS, 15.89 % higher than the Raw. The incorporation of SHC-IV further enhanced hydrolysis, acidogenesis, and methanogenesis, with the TC50 +SHC-IV achieving the highest improvement (7.61 %) compared to TC50 alone. Microbial diversity analysis revealed that TC and SHC-IV increased Chao1 and Shannon indices, indicating enhanced microbial richness and diversity. TC addition shifted the dominant methanogen from Methanosaeta to Methanobacterium, while SHC-IV enriched Syntrophomonas and Methanosarcina, promoting syntrophic interactions and optimizing the methanogenic pathway. Furthermore, SHC-IV addition enhanced the removal of TC, with the TC50 +SHC-IV group reaching the highest removal increase of 4.93 % compared to TC50 alone. These findings demonstrate that SHC-IV not only mitigates the environmental risks of TC in sludge but also enhances anaerobic digestion performance, offering a sustainable approach for in-plant sludge hydrothermal product utilization.
厌氧消化是有机物降解和高附加值产品回收的有效策略。虽然抗生素如四环素(TC)对厌氧消化的抑制作用是已知的,尽管已经探索了基于生物炭的载体来减轻这种抑制,但水茶同时去除抗生素和增强微生物活性的潜力仍不清楚。本研究以稻壳制备的污泥源水热炭(SHC-IV)为生物载体,提高了四环素(TC)污染污泥的厌氧消化性能。结果表明,适度添加TC (TC100)提高了甲烷产量,最大累积产率为44.97 mL/g·VS,比Raw提高15.89 %。SHC-IV的掺入进一步增强了水解、产酸和产甲烷,与单独TC50相比,TC50 +SHC-IV获得了最高的改善(7.61 %)。微生物多样性分析显示,TC和SHC-IV增加了Chao1和Shannon指数,表明微生物丰富度和多样性增强。TC的加入使优势产甲烷菌从甲烷osaeta向甲烷杆菌转移,而SHC-IV则使Syntrophomonas和Methanosarcina富集,促进了共生相互作用,优化了产甲烷途径。此外,添加SHC-IV可以促进TC的去除,其中TC50 +SHC-IV组的去除率最高,比单独添加TC50的去除率提高4.93 %。这些研究结果表明,SHC-IV不仅可以减轻污泥中TC的环境风险,还可以提高厌氧消化性能,为厂内污泥热液产物的可持续利用提供了途径。
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引用次数: 0
DFT investigation of heteronuclear bimetallic CrMPc (M=Mn, Co) monolayers for sensing VOCs with high selectivity 异核双金属CrMPc (M=Mn, Co)单分子膜对VOCs高选择性传感的DFT研究
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-15 DOI: 10.1016/j.jece.2026.121196
Junhui Li , Yifu Zhang , Gengfeng Deng , Huihui Xiong
Volatile organic compounds (VOCs) have emerged as one of the major atmospheric pollutants, posing serious threats to the ecological environment and human health. Consequently, the development of high-performance VOC gas sensors is of great importance. Based on density functional theory (DFT), this work systematically investigates the adsorption behaviors, electronic structures, and gas-sensing properties of five typical VOCs (C2H4, CH3Cl, C6H6, H2CO, and CH3OH) on two types of heteronuclear bimetallic phthalocyanine (CrMPc, M = Mn, Co) monolayers. Adsorption analysis reveals that CrMnPc and CrCoPc exhibit strong chemisorption toward C2H4, H2CO, and CH3OH, whereas physisorption dominates for C6H6 and CH3Cl. Furthermore, electronic structure analysis further elucidates the underlying mechanisms during adsorption, including charge transfer, orbital hybridization, and electron density distribution between the VOC molecules and the CrMPc substrate. Moreover, the adsorption strength towards target VOCs is significantly higher than that towards common interfering gases (N2, CO2, CH4), demonstrating excellent intrinsic selectivity. Finally, assessments of sensitivity and recovery time demonstrate that CrMnPc exhibits high responsiveness and suitable recovery kinetics towards C2H4, H2CO, and C6H6 across various temperatures, whereas CrCoPc is suitable for detecting H2CO, CH3OH, and C2H4 at moderate temperatures. Overall, these findings demonstrate the novel two-dimensional heteronuclear bimetallic phthalocyanines, CrMnPc and CrCoPc, hold great promise for VOC gas sensing applications, providing a theoretical foundation for the future design and development of high-performance, recyclable gas-sensing materials.
挥发性有机物(VOCs)已成为主要的大气污染物之一,对生态环境和人类健康构成严重威胁。因此,开发高性能VOC气体传感器具有十分重要的意义。基于密度泛函理论(DFT),系统研究了五种典型挥发性有机化合物(C2H4、CH3Cl、C6H6、H2CO和CH3OH)在两种异核双金属酞菁(CrMPc, M = Mn, Co)单分子膜上的吸附行为、电子结构和气敏性能。吸附分析表明,CrMnPc和CrCoPc对C2H4、H2CO和CH3OH具有较强的化学吸附作用,而对C6H6和CH3Cl具有较强的物理吸附作用。此外,电子结构分析进一步阐明了吸附过程中的潜在机制,包括VOC分子与CrMPc底物之间的电荷转移、轨道杂化和电子密度分布。对目标VOCs的吸附强度显著高于对常见干扰气体(N2、CO2、CH4)的吸附强度,表现出优异的本征选择性。最后,对灵敏度和恢复时间的评估表明,CrMnPc在不同温度下对C2H4、H2CO和C6H6具有较高的响应性和合适的恢复动力学,而CrCoPc则适合在中等温度下检测H2CO、CH3OH和C2H4。总的来说,这些发现表明,新型的二维异核双金属酞菁CrMnPc和CrCoPc在VOC气敏应用中具有很大的前景,为未来设计和开发高性能、可回收的气敏材料提供了理论基础。
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引用次数: 0
A regenerable thermo-responsive nanofiltration membrane with a molecularly anchored multilayer architecture for enhanced anti-scaling 一种具有分子锚定多层结构的可再生热响应纳滤膜,用于增强抗结垢性
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-15 DOI: 10.1016/j.jece.2026.121264
Chun Wang , Jialin Wei , Zhiyuan Qiao , Jingwen Chu , Feng Xu , Yang Ye , Haolong Xue , Dawei Ji , Jingjing Yan , Changfa Xiao
This study fabricated a thermally self-cleaning nanofiltration membrane through molecular design and multi-scale assembly. PNIPAM-PEI microgels, synthesized by grafting PNIPAM and PEI, were deposited on a PPTA ultrafiltration substrate via layer-by-layer self-assembly. The deposition cycles were systematically optimized, followed by interfacial polymerization to form a polyamide separation layer. Characterization confirmed that five deposition cycles yielded a compact thermo-responsive intermediate layer and resulted in an interpenetrating [PEMs-PNIPAM]-PA structure. The resultant composite NF membrane exhibited excellent separation performance, with rejections of CaCl2 and MgSO4 reaching 97.3 % and 98.7 %, respectively, at 25 ℃, along with intelligent thermo-responsive behavior. When heated above the LCST, dehydration and contraction of the PNIPAM core drove the expansion of PA layer pores, activating a “pore expansion” self-cleaning mechanism, with full structural regeneration upon cooling. A 180-hour long-term test verified that high-temperature backwashing at 60 ℃ effectively restored the flux and retention of the fouled membrane. This work offers a new strategy for developing smart nanofiltration membranes with self-cleaning capability.
本研究通过分子设计和多尺度组装制备了热自清洁纳滤膜。将PNIPAM和PEI接枝合成PNIPAM-PEI微凝胶,通过逐层自组装沉积在PPTA超滤基板上。系统地优化了沉积周期,然后进行界面聚合形成聚酰胺分离层。表征证实,五次沉积循环产生了致密的热响应中间层,并产生了互穿[pms - pnipam]-PA结构。复合膜在25℃条件下,CaCl2和MgSO4的去除率分别达到97.3% %和98.7% %,并具有智能的热响应行为。当加热到LCST以上时,PNIPAM芯的脱水和收缩驱动PA层孔隙的膨胀,激活“孔膨胀”自清洁机制,冷却后具有充分的结构再生。180小时的长期试验证明,60℃高温反冲洗能有效恢复污染膜的通量和截留。这项工作为开发具有自清洁能力的智能纳滤膜提供了一种新的策略。
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引用次数: 0
Sulfidation-engineered S-vacancy spinel NiCo2S4 nanowires on flexible substrate for enhanced photothermal CO2 reduction with high CO selectivity 柔性衬底上的硫化工程s空位尖晶石NiCo2S4纳米线,具有高CO选择性的增强光热CO2还原
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-15 DOI: 10.1016/j.jece.2026.121248
Lu Ruan, Yuanfei Gao, Zhengdao Li, Shuxian Xu, Luzi Yang, Xingjian Zhang, Jiping Shi, Haiquan Xie
The development of efficient photothermal catalysts for CO2 reduction into valuable fuels is crucial for sustainable energy utilization and environmental protection. Considering the advantageous properties of spinel-structured materials in photothermal catalytic reactions, vertically aligned VS-NiCo2S4 nanowires with sulfur-vacancy were synthesized on a sintered stainless steel fiber felt (SSFF). The catalyst was fabricated via sulfidation of NiCo2O4 nanowire precursors, simultaneously achieving structural transformation and S-vacancy introduction to enhance the performance of photothermal CO2 reduction. Sulfur substitution optimized the band structure by narrowing the bandgap and elevating the conduction band potential, thereby enhancing near-infrared light absorption and reducibility. Concurrently, the introduced S-vacancies generated abundant active sites, suppressed electron-hole recombination, promoted carrier separation, and facilitated proton-coupled electron transfer via stabilization of *COOH intermediate for selective CO generation. Furthermore, the flexible substrate prevented nanowire agglomeration, enhanced light harvesting via multiple scattering, and facilitated heat/electron transfer, thereby providing an ideal photothermal catalysis platform. Consequently, the VS-NiCo2S4 system achieved an impressive CO production rate of 694.7 μmol·m−2·h−1 with a selectivity of 92.1 %, representing a 29.4-fold enhancement over its NiCo2O4 precursor. This study demonstrates that defect engineering in spinel sulfides combined with rational three-dimensional substrate design, offers a promising strategy toward efficient and scalable photothermal CO2 conversion.
开发高效的光热催化剂将CO2还原为有价值的燃料,对于能源的可持续利用和环境保护至关重要。考虑到尖晶石结构材料在光热催化反应中的优越性能,在烧结不锈钢纤维毡(SSFF)上合成了具有硫空位的垂直排列VS-NiCo2S4纳米线。该催化剂通过NiCo2O4纳米线前驱体的硫化制备,同时实现了结构转变和s空位的引入,提高了光热还原CO2的性能。硫取代通过缩小带隙和提高导带电位来优化能带结构,从而增强近红外光的吸收和还原性。同时,引入的s -空位产生丰富的活性位点,抑制电子-空穴复合,促进载流子分离,并通过稳定*COOH中间体促进质子耦合电子转移,选择性生成CO。此外,柔性衬底防止了纳米线团聚,通过多次散射增强了光收集,促进了热/电子传递,从而提供了理想的光热催化平台。结果表明,VS-NiCo2S4体系的CO产率为694.7 μmol·m−2·h−1,选择性为92.1 %,比NiCo2O4前驱体提高了29.4倍。该研究表明,尖晶石硫化物的缺陷工程与合理的三维衬底设计相结合,为实现高效、可扩展的光热CO2转化提供了一种有前途的策略。
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引用次数: 0
A review of VOCs removal by cycled storage discharge plasma catalysis: Catalysts design, operation parameters, and applications 循环贮存放电等离子体催化去除挥发性有机化合物的研究进展:催化剂设计、运行参数及应用
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-15 DOI: 10.1016/j.jece.2026.121260
Amin Zhou , Huiqi Zheng , Ke Zhao , Haoyu Lian , Chuanyi Wang
The emission of volatile organic compounds (VOCs) has caused serious environmental pollution and threaten human health due to their toxic and carcinogenic nature. Plasma catalysis has been recognized as a promising technology to for VOCs removal, particularly the cycled storage-discharge (CSD) plasma catalysis, which can effectively overcome the high energy consumption associated with in-plasma catalysis and post-plasma catalysis systems. However, several critical challenges remain, such as the need to further improve removal efficiency and elucidate the unclear coupling mechanism. This review presents different types of plasma catalysis for VOCs removal, with the aim to provide a comprehensive understanding of the latest advancements in VOCs abatement by plasma catalysis. The plasma catalysis process is surveyed from three key aspects: (i) recent advances in plasma catalysis technologies based on catalyst configuration and operation modes of plasma; (ii) progress in VOCs removal by the CSD mode, focusing on catalyst design and operation parameters; and (iii) an exploration of the reaction mechanisms involved in VOCs removal, along with the future directions for mechanism investigation. Although significant attention has been devoted to VOCs removal by plasma catalysis, the reaction mechanism of VOCs oxidation remains a crucial challenge that deserves further investigation. This review is expected to provide theoretical reference for wide application of CSD mode of plasma catalysis for VOCs abatement in the future.
挥发性有机化合物(VOCs)由于其有毒和致癌的特性,已经造成了严重的环境污染,威胁着人类的健康。等离子体催化被认为是一种很有前途的去除VOCs的技术,特别是循环储放(CSD)等离子体催化,它可以有效地克服等离子体内催化和等离子体后催化系统所带来的高能耗。然而,一些关键的挑战仍然存在,例如需要进一步提高去除效率和阐明不明确的耦合机制。本文综述了不同类型的等离子体催化去除VOCs的方法,旨在全面了解等离子体催化去除VOCs的最新进展。从三个方面综述了等离子体催化过程:(1)基于催化剂配置和等离子体运行模式的等离子体催化技术的最新进展;(ii) CSD模式去除VOCs的进展,重点是催化剂设计和操作参数;(三)探讨挥发性有机化合物去除的反应机制,以及未来机制研究的方向。虽然等离子体催化去除挥发性有机化合物(VOCs)的研究得到了广泛的关注,但其氧化反应机理仍是一个值得进一步研究的重大挑战。该综述有望为今后等离子体催化CSD模式在VOCs减排中的广泛应用提供理论参考。
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引用次数: 0
Valorization of fly ash into hydrophobic mesoporous SiO₂ as a highly efficient and durable antifoaming agent for wet flue gas desulfurization 粉煤灰活化成疏水介孔sio2,作为一种高效、耐用的湿法烟气脱硫消泡剂
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-15 DOI: 10.1016/j.jece.2026.121274
Fei Wang , Xiaoyan Yan , Xiaoke Li , Jiangtao Meng , Yu Che , Jing Wang , Yuanyuan Zhang
In critical industrial processes such as wet flue gas desulfurization (WFGD), persistent foam formation poses a severe threat to process stability and operational efficiency. Conventional molecular antifoams face a fundamental paradox: they offer high initial efficiency but lack long-term durability. This trade-off arises because they are active initially but rapidly lose performance due to emulsification or adsorption. This study reports a novel “spike-reservoir” dual-functional composite antifoaming agent (HFS-AF) synthesized from industrial solid waste fly ash (FA). Through an optimized “mineral phase transformation-acid etching” protocol employing a Na₂CO₃-K₂CO₃ (3:1) composite activator and subsequent 20 % HCl etching, fly ash was successfully converted into high-purity mesoporous SiO₂ (HFS). The HFS exhibits a high specific surface area of 536 m²/g and a uniform pore diameter of 3.4 nm. After hydrophobic modification under optimal conditions (80 ℃, 6 h, 1:0.8), the material achieves a static water contact angle of 144.4°. Performance evaluations demonstrate that the HFS-AF composite system substantially outperforms commercial antifoaming agents, with its prolonged foam suppression time (17.5 min) representing a remarkable 71 % enhancement over commercial products (10.2 min). This performance leap is attributed to its dual-functional mechanism: the sharp edges of hydrophobic solid particles mechanically puncture foam lamellae, achieving instantaneous film rupture, while the high pore volume of 0.52 cm³ /g serves as a polyether “reservoir”, enabling sustained long-term release. This work provides a novel structural paradigm for designing advanced durable antifoaming materials and offers a cost-effective pathway for the high-value utilization of solid waste fly ash, achieving significant reduction in preparation cost.
在诸如湿法烟气脱硫(WFGD)等关键工业过程中,持续的泡沫形成对过程稳定性和运行效率构成严重威胁。传统的分子防泡沫塑料面临着一个根本的悖论:它们提供了很高的初始效率,但缺乏长期耐用性。这种权衡的出现是因为它们最初是有活性的,但由于乳化或吸附而迅速失去性能。本文报道了一种以工业固体废弃物飞灰(FA)为原料合成的新型“尖峰-储层”双功能复合消泡剂(HFS-AF)。采用Na₂CO₃-K₂CO₃(3:1)复合活化剂和20 % HCl蚀刻,采用优化的“矿物相变-酸蚀”工艺,成功地将粉煤灰转化为高纯度介孔sio2 (HFS)。HFS具有536 m²/g的高比表面积和3.4 nm的均匀孔径。在最佳条件下(80℃,6 h, 1:0.8)进行疏水改性后,材料的静态水接触角为144.4°。性能评估表明,HFS-AF复合体系大大优于商用消泡剂,其泡沫抑制时间延长(17.5 min),比商用产品(10.2 min)显著提高71 %。这种性能的飞跃归功于它的双重功能机制:疏水固体颗粒的锋利边缘机械地刺穿泡沫片层,实现瞬时薄膜破裂,而0.52 cm³ /g的高孔体积作为聚醚“储层”,实现持续的长期释放。本研究为设计先进耐用的消泡材料提供了一种新的结构范式,并为固废粉煤灰的高价值利用提供了一条经济有效的途径,实现了制备成本的显著降低。
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引用次数: 0
A review of biological treatment strategies for antibiotic resistance genes in livestock wastewater: Challenges, advances, and future directions 畜禽废水中抗生素耐药基因的生物处理策略综述:挑战、进展和未来方向
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-15 DOI: 10.1016/j.jece.2026.121234
Lianggang Tang , Lei Liu , Liang Xie , Xingtao Miao , Yingqi Zhou , Wenbin Liu
The extensive use of antibiotics in animal husbandry has led to wastewater becoming an important reservoir of antibiotic resistance genes (ARGs), posing a serious threat to public health. However, at present, there is a lack of research summarizing and analyzing the occurrence and removal mechanisms of ARGs in these wastewaters from the perspective of biological wastewater treatment, which makes it difficult to effectively formulate strategies to control these pollutants. Although traditional biological treatment processes can effectively remove organic pollutants, they often show inconsistent and insufficient performance in removing ARGs. More crucially, these systems may become hotspots for horizontal gene transfer (HGT), driven by the co-selection pressure of mobile genetic elements and heavy metals and residual antibiotics, thereby amplifying the spread of ARGs. This article reviews the current research status of ARGs biological treatment technology in livestock wastewater. The effectiveness and limitations of traditional methods (such as anaerobic digestion and constructed wetlands) and emerging treatment methods (such as aerobic granular sludge, microalgae systems, and biochar enhancement) were systematically evaluated. The complex interactions among microbial community dynamics, adsorption, degradation and HGT in determining the fate of ARGs were also discussed. This article clarifies the challenges and difficulties faced in removing ARGs from livestock wastewater and proposes future research directions.
畜牧业中抗生素的广泛使用导致废水成为抗生素耐药基因(ARGs)的重要储存库,对公众健康构成严重威胁。然而,目前缺乏从废水生物处理角度对这些废水中ARGs的发生和去除机理进行总结和分析的研究,难以有效制定控制这些污染物的策略。传统的生物处理工艺虽然可以有效去除有机污染物,但在去除ARGs方面往往表现出不一致和不足的性能。更重要的是,这些系统可能成为水平基因转移(HGT)的热点,在移动遗传元件、重金属和残留抗生素的共同选择压力的驱动下,从而放大ARGs的传播。本文综述了ARGs生物处理畜禽废水技术的研究现状。系统评价了传统方法(如厌氧消化和人工湿地)和新兴处理方法(如好氧颗粒污泥、微藻系统和生物炭强化)的有效性和局限性。讨论了微生物群落动态、吸附、降解和HGT之间复杂的相互作用对ARGs命运的影响。本文阐述了从畜禽废水中去除ARGs面临的挑战和困难,并提出了未来的研究方向。
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引用次数: 0
Environmental risks and upcycling potential in ternary geopolymer development for oily sludge pyrolysis byproducts 含油污泥热解副产物三元地聚合物开发的环境风险与升级利用潜力
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-15 DOI: 10.1016/j.jece.2026.121265
Chenxu Zhong , Chujun Luan , Xuan Guo , Fawei Lin , Jingwei Li , Beibei Yan , Zhanjun Cheng , Eminov Ashraf Mamurovich , Bigaliev Aitkhazha Bigalievich , Guanyi Chen
This study develops a ternary geopolymer system combining fly ash (FA), pyrolysis residue (PR), and ground granulated blast furnace slag (GGBS), designed to simultaneously enhance solidification performance and resource utilization. Unlike conventional binary FA-GGBS or PR-GGBS systems, the deliberate incorporation of PR (silica-rich, lamellar, and organically coated) enables complementary reactivity and microstructural densification, yielding a more robust immobilization matrix. Using a one-step dry-mix alkali activation route, hazardous FA and PR were converted into structural materials exhibiting high contaminant stabilization, including > 99 % Pb immobilization, while maintaining strong early mechanical strength (47.85 MPa at 7 days). Durability testing confirmed resistance to aggressive environments, even at 30 % waste substitution. Life-cycle analysis demonstrated reduced carbon emissions and net economic advantages relative to conventional disposal-based approaches. Mechanistic analysis indicates that the ternary system promotes synergistic stabilization through compact C-(A)-S-H gel formation, physical encapsulation, ion exchange, and metal–silicate bonding. These findings demonstrate that the FA-PR-GGBS ternary framework provides a scalable, low-carbon pathway that simultaneously addresses hazardous waste management and infrastructure sustainability.
本研究开发了一种由粉煤灰(FA)、热解渣(PR)和磨粒高炉渣(GGBS)组成的三元地聚合物体系,旨在同时提高固化性能和资源利用率。与传统的二元FA-GGBS或PR- ggbs系统不同,PR(富含二氧化硅、层状和有机涂层)的刻意掺入可以实现互补的反应性和微观结构致密化,从而产生更坚固的固定基质。采用一步干混碱活化法,将有害FA和PR转化为具有高污染物稳定性的结构材料,包括>; 99 % Pb固定化,同时保持较强的早期机械强度(7天47.85 MPa)。耐久性测试证实耐腐蚀性环境,即使在30 %的废物替代。生命周期分析表明,与传统的基于处置的方法相比,减少了碳排放和净经济优势。机理分析表明,三元体系通过致密的C-(A)- s - h凝胶形成、物理包封、离子交换和金属-硅酸盐键合促进协同稳定。这些发现表明,FA-PR-GGBS三元框架提供了一种可扩展的低碳途径,同时解决了危险废物管理和基础设施可持续性问题。
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引用次数: 0
Enhancing the efficiency of catalytic transfer hydrogenation in the production of γ-valerolactone from biomass with metal-organic frameworks supported by ruthenium-substituted phosphovanadomolybdic acid 钌取代磷钒钼酸负载金属有机骨架催化加氢制备γ-戊内酯的研究
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-15 DOI: 10.1016/j.jece.2026.121271
He Wan , Fanqi Yan , Yue Zhao , Yongwei Han , Zhong Sun , Xixin Duan
Biomass is a promising raw material to prepare green solvent of γ-valerolactone (GVL). A series of Ru-substituted vanadium-containing polyoxometalates (POMs) of Run/3H4-nPMo11VO40 (n = 1, 2, 3, 4) and Run/3H5-n PMo10V2O40 (n = 1, 2, 3, 4, 5) were prepared, which were loaded on metal organic frameworks (MOFs) to afford POMs@MOF with adjusting strong oxidizing abilities. This paper focused on the effects of POMs@MOF on improving the yield and selectivity of GVL in a green system of formic acid (FA) and water. When cellulose, glucose, and levulinic acid (LA) were used as substrates, the yields of GVL were 43.2 %, 69.7 %, and 98.3 % with the selectivity of 48.0 %, 71.9 %, and 99.3 %, respectively. The results indicate that the strong oxidizing ability of POMs favors the conversion of biomass to GVL. The proposed catalytic system greatly reduces the use of noble metal Ru while enhancing the catalytic transfer hydrogenation performances. The adjustment of the proportion of Ru in POMs can provide efficient and promising catalytic systems for one-pot production of GVL from biomass with different structures.
生物质是制备γ-戊内酯(GVL)绿色溶剂的重要原料。制备了Run/3H4-nPMo11VO40 (n = 1,2,3,4)和Run/3H5-n PMo10V2O40 (n = 1,2,3,4,5)的一系列ru取代含钒多金属氧酸盐(POMs),并将其负载在金属有机骨架(mfs)上,获得了具有调节强氧化能力的POMs@MOF。研究了POMs@MOF在甲酸-水绿色体系中对提高GVL收率和选择性的影响。以纤维素、葡萄糖和乙酰丙酸(LA)为底物时,GVL的产率分别为43.2% %、69.7% %和98.3% %,选择性分别为48.0% %、71.9 %和99.3 %。结果表明,pom具有较强的氧化能力,有利于生物质转化为GVL。所提出的催化体系大大减少了贵金属Ru的使用,同时提高了催化转移加氢性能。调整POMs中Ru的比例可以为不同结构的生物质一锅制GVL提供高效的催化体系。
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引用次数: 0
Ionic liquid-modified hollow microspheres of tartaric acid-anion intercalated LDH in PIM-1 membranes for superior CO2/N2 separation 离子液体修饰酒石酸中空微球-阴离子嵌入LDH在PIM-1膜上的优越CO2/N2分离
IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-01-15 DOI: 10.1016/j.jece.2026.121277
Caifeng Xia , Siyuan Liu , Qikang Yin , Sen Liu , Bo Liao , Shuxian Wei , Zhaojie Wang , Zhe Sun , Xiaoqing Lu
The performance of mixed matrix membranes (MMMs) depends largely on the structure and composition of incorporated nanofillers. However, it remains challenging to achieve efficient separation performance with uniform filler dispersion and strong interfacial compatibility within the polymer matrix. In this study, an ionic liquid-modified hollow microsphere of tartaric acid anion-intercalated layered double hydroxide (IL@HMS TA-LDH) was designed and embedded into a PIM-1 matrix to fabricate IL@HMS TA-LDH/PIM-1 MMMs for efficient CO2 separation. The hollow microstructure and anion-rich interlayers of LDH provide multiple facilitated transport pathways for CO2 significantly enhancing both permeability and selectivity. Experimental and theoretical calculation results confirm that IL modification on HMS TA-LDH not only improved the interfacial compatibility between the polymer and the filler but also enhanced CO2 affinity and the CO2/N2 selectivity. The resulting MMMs surpassed the 2019 Robeson upper bound and showed good stability. The separation efficiency of the optimal 5.0 % IL@HMS TA-LDH/PIM-1 MMMs was the best (CO2 permeability was 8550.73 ± 367.54 Barrer, CO2/N2 selectivity was 40.75 ± 1.83), outperforming most of the other reported MMMs. This work offers a new strategy for designing high-performance CO2 capture membranes by combining hollow-structured LDH with functionalized ionic liquids.
混合基质膜(MMMs)的性能在很大程度上取决于纳米填料的结构和组成。然而,如何在聚合物基体内实现均匀分散和强界面相容性的高效分离仍然是一个挑战。本研究设计了一种离子液体修饰的酒石酸阴离子插入层状双氢氧化物中空微球(IL@HMS TA-LDH),并将其嵌入到PIM-1基体中,制备了IL@HMS TA-LDH/PIM-1 mmmm,用于高效的CO2分离。LDH的中空结构和富含阴离子的中间层为CO2提供了多种便利的运输途径,显著提高了其渗透性和选择性。实验和理论计算结果证实,IL对HMS TA-LDH的改性不仅改善了聚合物与填料之间的界面相容性,而且提高了CO2亲和力和CO2/N2选择性。所得到的MMMs超过了2019年罗布森上限,并表现出良好的稳定性。最优的5.0 % IL@HMS TA-LDH/PIM-1 MMMs的分离效率最高(CO2渗透率为8550.73 ± 367.54 Barrer, CO2/N2选择性为40.75 ± 1.83),优于其他大多数已报道的MMMs。本研究通过将空心结构LDH与功能化离子液体相结合,为设计高性能CO2捕集膜提供了一种新的策略。
{"title":"Ionic liquid-modified hollow microspheres of tartaric acid-anion intercalated LDH in PIM-1 membranes for superior CO2/N2 separation","authors":"Caifeng Xia ,&nbsp;Siyuan Liu ,&nbsp;Qikang Yin ,&nbsp;Sen Liu ,&nbsp;Bo Liao ,&nbsp;Shuxian Wei ,&nbsp;Zhaojie Wang ,&nbsp;Zhe Sun ,&nbsp;Xiaoqing Lu","doi":"10.1016/j.jece.2026.121277","DOIUrl":"10.1016/j.jece.2026.121277","url":null,"abstract":"<div><div>The performance of mixed matrix membranes (MMMs) depends largely on the structure and composition of incorporated nanofillers. However, it remains challenging to achieve efficient separation performance with uniform filler dispersion and strong interfacial compatibility within the polymer matrix. In this study, an ionic liquid-modified hollow microsphere of tartaric acid anion-intercalated layered double hydroxide (IL@HMS TA-LDH) was designed and embedded into a PIM-1 matrix to fabricate IL@HMS TA-LDH/PIM-1 MMMs for efficient CO<sub>2</sub> separation. The hollow microstructure and anion-rich interlayers of LDH provide multiple facilitated transport pathways for CO<sub>2</sub> significantly enhancing both permeability and selectivity. Experimental and theoretical calculation results confirm that IL modification on HMS TA-LDH not only improved the interfacial compatibility between the polymer and the filler but also enhanced CO<sub>2</sub> affinity and the CO<sub>2</sub>/N<sub>2</sub> selectivity. The resulting MMMs surpassed the 2019 Robeson upper bound and showed good stability. The separation efficiency of the optimal 5.0 % IL@HMS TA-LDH/PIM-1 MMMs was the best (CO<sub>2</sub> permeability was 8550.73 ± 367.54 Barrer, CO<sub>2</sub>/N<sub>2</sub> selectivity was 40.75 ± 1.83), outperforming most of the other reported MMMs. This work offers a new strategy for designing high-performance CO<sub>2</sub> capture membranes by combining hollow-structured LDH with functionalized ionic liquids.</div></div>","PeriodicalId":15759,"journal":{"name":"Journal of Environmental Chemical Engineering","volume":"14 2","pages":"Article 121277"},"PeriodicalIF":7.2,"publicationDate":"2026-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145981480","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Journal of Environmental Chemical Engineering
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