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Sustainable capture and photocatalytic degradation of organic pollutants by high-swelling cyclodextrin polymer loaded with TiO2 nanoparticles 负载TiO2纳米颗粒的高溶胀环糊精聚合物可持续捕获和光催化降解有机污染物
IF 9.2 2区 工程技术 Q1 ENERGY & FUELS Pub Date : 2025-12-24 DOI: 10.1016/j.susmat.2025.e01831
Kai Zhang , Zhaoxin Zhang , Ningning Cao , Linji Li , Ningyan Peng , Yongli Shi , Guofei Dai , Xiaojin Zhang
Abstract
Photocatalytic degradation provides a promising sustainable solution for water purification, but its effectiveness is often limited by the low utilization efficiency of photogenerated reactive oxygen species (ROS). Although organic coatings such as fluorinated porous cyclodextrin polymers can adsorb target pollutants near the photocatalyst surfaces to enhance ROS efficiency and resist ROS attack, their hydrophobicity may limit the adsorption and degradation of hydrophilic organic pollutants. Here, we report a novel core-shell photocatalyst (His-CDP-TiO2) prepared by a simple synthesis process that encapsulates TiO2 nanoparticles in a high-swelling cyclodextrin polymer (His-CDP). This design utilizes the exceptional broad-spectrum pollutant enrichment ability of His-CDP hydrophilic-hydrophobic dual-functional network to rapidly concentrate pollutants near catalytic TiO2 core sites. This localized enhancement significantly improves the interfacial ROS utilization efficiency and promotes efficient “capture-and-degradation” process. Therefore, His-CDP-TiO2 exhibits significantly accelerated photodegradation kinetics towards hydrophilic/hydrophobic organic pollutants. For example, it degraded over 99 % of bisphenol A (BPA) within 180 min, with a degradation rate constant (0.025 min−1) 4.4 times higher than unmodified TiO2. The photodegradation pathway of BPA was elucidated by identifying and quantifying the oxidation intermediates generated by His-CDP-TiO2.
摘要光催化降解为水净化提供了一种很有前景的可持续解决方案,但其效果往往受到光生活性氧(ROS)利用效率低的限制。虽然氟化多孔环糊精聚合物等有机涂层可以吸附光催化剂表面附近的目标污染物,提高ROS效率,抵抗ROS的攻击,但其疏水性可能会限制亲水有机污染物的吸附和降解。在这里,我们报道了一种新型的核壳光催化剂(His-CDP-TiO2),该催化剂通过简单的合成工艺将TiO2纳米颗粒封装在高膨胀的环糊精聚合物(His-CDP)中。该设计利用His-CDP亲疏水双功能网络独特的广谱污染物富集能力,在催化TiO2核心位点附近快速富集污染物。这种局部增强显著提高了界面ROS的利用效率,促进了高效的“捕获-降解”过程。因此,His-CDP-TiO2对亲水/疏水有机污染物表现出明显加速的光降解动力学。例如,它在180分钟内降解了99%以上的双酚A (BPA),降解速率常数(0.025 min−1)是未改性TiO2的4.4倍。通过鉴定和定量His-CDP-TiO2生成的氧化中间体,阐明了BPA的光降解途径。
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引用次数: 0
Plasmonic–heterojunction nanostructures: Mechanistic design for photocatalysis, energy conversion, and advanced biosensing 等离子体-异质结纳米结构:光催化、能量转换和先进生物传感的机械设计
IF 9.2 2区 工程技术 Q1 ENERGY & FUELS Pub Date : 2025-12-24 DOI: 10.1016/j.susmat.2025.e01833
Yuan-Fong Chau Chou , Sy-Hann Chen , Abdul Hanif Mahadi , Roshan Thotagamuge , Chee Ming Lim , Muhammad Raziq Rahimi Kooh
Plasmonic-heterojunction photocatalysts represent a rapidly advancing frontier in photocatalysis, merging the strong light–matter interactions of plasmonic nanostructures with the superior charge-separation efficiency of semiconductor heterojunctions. This synergistic integration facilitates hot-carrier generation, near-field amplification, and localized photothermal heating, while the heterojunction interface guides directional carrier transport and preserves redox potentials. Consequently, these systems achieve broadband solar harvesting, extended charge-carrier lifetimes, and enhanced selectivity in catalytic reactions. This review provides a comprehensive overview of plasmon-enhanced photocatalysis, commencing with the fundamental mechanisms of plasmon–exciton coupling, hot carrier injection, near-field interactions, and photothermal effects. We subsequently explore diverse materials platforms, including noble metals, earth-abundant alternatives, doped oxides, refractory nitrides, 2D materials, and hybrid frameworks such as MOFs and perovskites. Architectures such as Schottky, type-II, Z- and S-schemes, core–shells, cascades, and hierarchical systems are examined to elucidate how design dictates charge dynamics. Applications are reviewed for sustainable energy conversion (hydrogen evolution, CO₂ reduction, solar fuels), environmental remediation (pollutant degradation, wastewater treatment) and sensing (photoelectrochemical sensors, SERS, wearable platforms). Finally, we propose design principles and identify emerging frontiers, including scalable fabrication, AI-guided materials discovery, and quantum plasmonics. By bridging nanophotonics, catalysis, and device engineering, plasmonic heterojunctions emerge as multifunctional systems poised to drive the next generation of sustainable technologies.
等离子体-异质结光催化剂融合了等离子体纳米结构的强光-物质相互作用和半导体异质结优越的电荷分离效率,是光催化领域一个快速发展的前沿领域。这种协同集成促进了热载流子的产生、近场放大和局部光热加热,而异质结界面引导定向载流子传输并保持氧化还原电位。因此,这些系统实现了宽带太阳能收集,延长了载流子寿命,并提高了催化反应的选择性。本文从等离子体-激子耦合、热载流子注入、近场相互作用和光热效应的基本机制开始,对等离子体增强光催化进行了全面的综述。我们随后探索了不同的材料平台,包括贵金属,地球丰富的替代品,掺杂氧化物,耐火氮化物,二维材料和混合框架,如mof和钙钛矿。架构,如肖特基,ii型,Z-和s -方案,核壳,级联,和分层系统进行检查,以阐明如何设计决定电荷动力学。综述了可持续能源转换(析氢、CO 2减排、太阳能燃料)、环境修复(污染物降解、废水处理)和传感(光电化学传感器、SERS、可穿戴平台)的应用。最后,我们提出了设计原则并确定了新兴领域,包括可扩展制造,人工智能引导材料发现和量子等离子体。通过桥接纳米光子学、催化和器件工程,等离子异质结作为多功能系统出现,有望推动下一代可持续技术。
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引用次数: 0
Recent advances in nanostructured boron nitride based flame retardant composites: A comprehensive review 纳米结构氮化硼基阻燃复合材料的研究进展
IF 9.2 2区 工程技术 Q1 ENERGY & FUELS Pub Date : 2025-12-23 DOI: 10.1016/j.susmat.2025.e01827
K. Deepthi Jayan , Kalim Deshmukh
With formerly unattainable control over material properties at the nanoscale, nanotechnology has emerged as a paradigm shift in materials research. Given the increasing demand for fire-resistant materials in industries, the use of nanomaterials in flame-retardant composites has garnered significant attention among their many other uses. The nanostructured boron nitride (BN) is a potential candidate in this area since it possesses outstanding structural and chemical properties and its two-dimensional (2D) structure endows them with thermal stability, high surface area, and natural flame resistance making them extremely valuable for fire safety improvement in many materials. In recent years, progress in the synthesis, functionalization, and use of nanostructured BN in flame retardant composites cast new light on the fundamental processes that underlie their flame-retardant properties but also triggered the creation of new, high-performance flame-retardant materials. This review provides an integral overview of the most recent advancements in nanostructured BN-based flame-retardant composites, systematically exploring the synthesis routes, properties, characterization methods, and flame retardancy mechanisms. The review explores the underlying principles of the flame-resistant BN-based composites, emphasizing their versatile applications in different industries highlighting their vast potential as next-generation flame retardants. The future trends and challenges associated with the extensive utilization of the nanostructured BN in flame retardant applications are briefed. With a detailed description of the state-of-the-art in nanostructured BN with flame-retardant composites, the current review intends to promote research activities in this emerging area leading to the progress of next-generation sustainable flame-retardant materials with excellent performance.
由于以前无法在纳米尺度上控制材料的特性,纳米技术已经成为材料研究的一个范式转变。鉴于工业对耐火材料的需求日益增加,纳米材料在阻燃复合材料中的应用在其许多其他用途中引起了极大的关注。纳米结构的氮化硼(BN)是这一领域的潜在候选者,因为它具有出色的结构和化学性质,其二维(2D)结构赋予它们热稳定性,高表面积和天然阻燃性,使它们在许多材料的消防安全改善方面非常有价值。近年来,纳米结构BN在阻燃复合材料中的合成、功能化和应用方面的进展,使人们对其阻燃性能的基本过程有了新的认识,同时也引发了新型高性能阻燃材料的创造。本文综述了纳米结构bn基阻燃复合材料的最新进展,系统地探讨了合成路线、性能、表征方法和阻燃机理。综述探讨了阻燃bn基复合材料的基本原理,强调了其在不同行业的广泛应用,突出了其作为下一代阻燃剂的巨大潜力。简要介绍了纳米结构BN在阻燃应用中广泛应用的未来趋势和挑战。通过对纳米结构BN阻燃复合材料最新进展的详细描述,本文旨在促进这一新兴领域的研究活动,从而开发出性能优异的下一代可持续阻燃材料。
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引用次数: 0
A sustainable solution for lithium-air batteries: Green polymer membrane with gradient pores for selective O₂ transport in humid air 锂空气电池的可持续解决方案:具有梯度孔的绿色聚合物膜,可在潮湿空气中选择性输送O₂
IF 9.2 2区 工程技术 Q1 ENERGY & FUELS Pub Date : 2025-12-23 DOI: 10.1016/j.susmat.2025.e01832
Wei Yuan, Hong Sun, Jie Li, Mingfu Yu, Jiaxin Pang, Liqiang Cui
The employment of green polymer membranes has emerged as a pivotal component in the advancement of the sustainability and performance of lithium-air batteries (LABs). This development offers an eco-friendly option in comparison to conventional lithium-ion batteries by LABs. The present paper sets out an innovative approach to developing green polymer membranes, namely oxygen selective membranes (O2SM), with an asymmetric structure comprising a surface macroporous layer (9.85 μm) and a dense bottom layer (1.5 μm). Prepared via a dry-wet phase transformation method, the O₂SM exhibits a superhydrophobic barrier (static contact angle of 100.19°), excellent water vapour barrier capability (flux of 330.7 g/cm2·24 h at 70 % RH) and ionic conductivity of 4.18 × 10−2 S/m. Under RH = 30 % conditions, the O₂/H₂O selectivity coefficient α of the O₂SM is 1.13. Even under RH = 70 % conditions, α is 0.88. When applied to lithium-air batteries, the batteries with the help of the O₂SM increased cycle life by 368 % (from 25 to 117 cycles), boosted specific capacity by 41.1 % (from 3590 to 5065 mAh/g) and reduced overpotential by 7.7 % (from 1.30 to 1.20 V). By addressing these challenges, green polymer membrane hold the potential to transform energy storage technologies, thereby supporting global energy transitions and facilitating a future that is more sustainable and energy-efficient.
绿色聚合物膜的使用已经成为锂空气电池可持续性和性能进步的关键组成部分(实验室)。与实验室的传统锂离子电池相比,这一发展提供了一种环保的选择。本文提出了一种开发绿色聚合物膜的创新方法,即氧选择膜(O2SM),其不对称结构由表面大孔层(9.85 μm)和致密底层(1.5 μm)组成。通过干湿相变法制备的O₂SM具有超疏水屏障(静态接触角为100.19°),优异的水蒸气屏障性能(在70% RH下通量为330.7 g/cm2·24 h),离子电导率为4.18 × 10−2 S/m。在RH = 30%的条件下,O₂/H₂O选择性系数α为1.13。即使在RH = 70%的条件下,α也为0.88。当应用于锂空气电池时,O₂SM电池的循环寿命延长了368%(从25次循环到117次循环),比容量提高了41.1%(从3590 mAh/g到5065 mAh/g),过电位降低了7.7%(从1.30 V到1.20 V)。通过解决这些挑战,绿色聚合物膜具有改变储能技术的潜力,从而支持全球能源转型,促进更加可持续和节能的未来。
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引用次数: 0
A terrain-adaptive soft robot with closed-loop sensing and control 一种具有闭环传感与控制的地形自适应软机器人
IF 9.2 2区 工程技术 Q1 ENERGY & FUELS Pub Date : 2025-12-22 DOI: 10.1016/j.susmat.2025.e01828
Zihan Wan , Sicheng Chen , Haibin Gao , Zhilin Yu , Li Xiang , Lei Yang , Wenling Zhang
In recent years, soft robotics have emerged as a prominent area of research, offering novel solutions to real-world challenges. However, enabling soft robots to achieve spontaneous terrain adaptation while maintaining stable motion remains a serious challenge. To address this problem, we propose a highly integrated soft robot that can recognize terrain features and autonomously adjust gait parameters through closed-loop sensing and control. The robot's mechanical design combines Kresling origami construction with flexible materials and a foot design with an asymmetrical structure for smooth transitions in the 0–0.103 BL/s speed range. The body-embedded flexible resistive sensor senses the body's motion state in real time and feeds the data as input to the machine learning model, achieving an accuracy of 98.69 % in terrain classification (flat, grass, and rock). The machine learning model results are used to adjust the motion frequency of the motion module to achieve adaptive motion. The fusion of advanced machinery and closed-loop control provides a robust framework for soft robots operating in complex, dynamic environments.
近年来,软机器人已成为一个突出的研究领域,为现实世界的挑战提供了新颖的解决方案。然而,使软体机器人在保持稳定运动的同时实现自发的地形适应仍然是一个严峻的挑战。为了解决这一问题,我们提出了一种高度集成的软机器人,它可以通过闭环传感和控制来识别地形特征并自主调整步态参数。机器人的机械设计结合了Kresling折纸结构和柔性材料,以及不对称结构的脚设计,以便在0-0.103 BL/s的速度范围内平稳过渡。嵌入身体的柔性电阻传感器实时感知身体的运动状态,并将数据作为输入输入到机器学习模型中,在地形分类(平坦、草地和岩石)方面实现了98.69%的准确率。利用机器学习模型的结果调整运动模块的运动频率,实现自适应运动。先进机械和闭环控制的融合为软机器人在复杂动态环境中运行提供了一个强大的框架。
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引用次数: 0
Advanced high entropy LDHs electrocatalysts: Synthesis and performance enhancement strategies for alkaline oxygen evolution reaction 新型高熵LDHs电催化剂的合成及碱析氧反应性能增强策略
IF 9.2 2区 工程技术 Q1 ENERGY & FUELS Pub Date : 2025-12-22 DOI: 10.1016/j.susmat.2025.e01829
Shuang Yin, Sheng Fu, Yibo Wang, Rongda Zhao, Liang Liu
High-entropy layered double hydroxides (HE-LDHs) are widely used as oxygen evolution catalysts due to their elemental diversity, lattice distortion and excellent stability. The cocktail effect and exquisite synthesis technology have made the customization of materials possible in recent years. This review centers on the effective synthesis strategies of HE-LDHs and their recent application progress in the alkaline oxygen evolution reaction (OER). Furthermore, it also explores performance enhancement strategies for HE-LDHs, including surface modification by doping, exfoliation of layered structures, defect engineering, and heterojunction construction. Finally, it proposes future perspectives for HE-LDHs, which provides valuable insights and references for researchers to obtain the next-generation OER materials.
高熵层状双氢氧化物(HE-LDHs)因其元素多样性、晶格畸变和优异的稳定性而被广泛用作析氧催化剂。近年来,鸡尾酒效应和精湛的合成技术使材料的定制成为可能。本文综述了HE-LDHs的有效合成策略及其在碱性析氧反应(OER)中的应用进展。此外,本文还探讨了HE-LDHs的性能增强策略,包括掺杂表面改性、层状结构剥离、缺陷工程和异质结构建。最后,提出了HE-LDHs的未来展望,为研究人员获得下一代OER材料提供了有价值的见解和参考。
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引用次数: 0
Solar driven photocatalytic glycerol and glucose reforming via noble metals free BiOX (X = Cl, Br, I)-TiO2 composites 利用不含贵金属的BiOX (X = Cl, Br, I)-TiO2复合材料进行光催化甘油和葡萄糖重整
IF 9.2 2区 工程技术 Q1 ENERGY & FUELS Pub Date : 2025-12-21 DOI: 10.1016/j.susmat.2025.e01825
Tayyaba Kanwal , Vittorio Loddo , Claudio Maria Pecoraro , Giovanni Palmisano , Sarah Hamdan , Zhe Wang , Israa Othman , Leonardo Palmisano , Marianna Bellardita
Recent research on the valorization of biomass has received a lot of interest as it allows the obtaining of products with high added value. In this regard, this study explores aerobic and anaerobic heterogeneous photocatalytic partial oxidation under both UV and simulated solar irradiation of glycerol and glucose in aqueous medium using bismuth oxyhalide-based photocatalysts BiOX (X = Cl, Br, I). Moreover, noble metal-free BiOX-TiO2 (P25) composites were prepared through a simple ball milling procedure. Both the formation of partial oxidation compounds, namely 1,3-dihydroxyacetone, glyceraldehyde and glycolic acid from glycerol and arabinose and formic acid from glucose in solution, and the production of CO2 and H2 in the gas phase, were followed. Pure BiOBr and BiOCl proved to be more effective than bare TiO2 P25 (one of the most used and studied photocatalysts) affording a higher selectivity  towards high added value products whilst the composites samples displayed high glycerol conversion values that reached 62 %. Particularly noteworthy was the effectiveness of BiOCl-P25 and BiOBr-P25 samples containing 5 and 7 wt% of BiOCl or BiOBr with respect to P25, in promoting also H2 formation under simulated sunlight irradiation and without the presence of noble metal species such as Pt. To the best of our knowledge, BiOX-TiO2 photocatalysts have never been used for the photoreforming of glycerol and glucose.
近年来,生物质的增值研究引起了人们的广泛关注,因为它可以获得高附加值的产品。为此,本研究利用氧卤化铋基光催化剂BiOX (X = Cl, Br, I),探索了在紫外和模拟太阳照射下,甘油和葡萄糖在水介质中的好氧和厌氧非均相光催化部分氧化。此外,通过简单的球磨工艺制备了无贵金属BiOX-TiO2 (P25)复合材料。在溶液中由甘油生成1,3-二羟基丙酮、甘油醛和乙醇酸,由葡萄糖生成阿拉伯糖和甲酸,并在气相中生成CO2和H2。事实证明,纯BiOBr和BiOCl比裸TiO2 P25(最常用和研究的光催化剂之一)更有效,对高附加值产品具有更高的选择性,而复合样品的甘油转化率高达62%。特别值得注意的是,在模拟阳光照射下,在没有贵金属(如Pt)存在的情况下,含有5%和7% BiOCl或BiOBr(相对于P25)的BiOCl-P25和BiOBr-P25样品在促进H2形成方面的有效性。据我们所知,BiOX-TiO2光催化剂从未用于甘油和葡萄糖的光转化。
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引用次数: 0
Employing diverse machine learning approaches to estimate the achievable bio-oil yield from sustainable biomass sources 采用不同的机器学习方法来估计可持续生物质资源可实现的生物油产量
IF 9.2 2区 工程技术 Q1 ENERGY & FUELS Pub Date : 2025-12-20 DOI: 10.1016/j.susmat.2025.e01823
Mohsen Karimi , Mohammad Shirzad , Behzad Vaferi
The construction of a process to produce bio-oil from biomass pyrolysis, as well as optimizing and controlling its operation, requires accurate prediction of yield under varying process conditions and feedstock properties. The existing models often fail to capture the complex relationship between bio-oil yield and feedstock properties and operating parameters. This study applies three well-known machine learning (ML) classes, i.e., adaptive neuro-fuzzy inference systems (ANFIS), artificial neural networks, and least-squares support vector regression to predict the bio-oil yield. 419 sets of experimental measurements about the achievable bio-oil yield from 40 biomass types at a wide range of pyrolysis temperature, heating rate, residence time, and gas flow rate are used for training these intelligent models and monitoring the reliability of their simulation performance. The relevancy test approved that the gas flow rate and heating rate, with the Pearson correlation coefficients of 0.392 and − 0.202, have the highest impact on the bio-oil yield. The statistical accuracy monitoring of the ML models confirmed that the ANFIS model outperformed all alternatives, achieving the mean absolute error (MAE), root mean square error (RMSE), absolute average relative deviation (AARD), and correlation coefficient (R) of 2.18, 3.69, 6.45 %, and 0.95541, respectively. This outstanding simulation performance of the ANFIS model is related to its hybrid architecture that integrates interpretable fuzzy rules with artificial neural network adaptability. The applicability domain investigation identifies seven outliers and one out-of-leverage sample among the experimental databank.
构建生物质热解生产生物油的工艺,并对其操作进行优化和控制,需要对不同工艺条件和原料性质下的产量进行准确预测。现有的模型往往不能捕捉生物油产量与原料性质和操作参数之间的复杂关系。本研究应用了三种著名的机器学习(ML)类,即自适应神经模糊推理系统(ANFIS)、人工神经网络和最小二乘支持向量回归来预测生物油产量。通过对40种生物质在不同热解温度、加热速率、停留时间和气体流速下可实现的生物油产率的419组实验测量,对这些智能模型进行了训练,并监测其模拟性能的可靠性。相关性检验表明,气体流速和升温速率对生物油收率的影响最大,Pearson相关系数分别为0.392和- 0.202。对ML模型的统计精度监测证实,ANFIS模型优于所有替代模型,平均绝对误差(MAE)、均方根误差(RMSE)、绝对平均相对偏差(AARD)和相关系数(R)分别为2.18、3.69、6.45%和0.95541。ANFIS模型出色的仿真性能与其融合了可解释模糊规则和人工神经网络自适应性的混合体系结构有关。适用性领域调查确定了实验数据库中的7个异常值和1个非杠杆样本。
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引用次数: 0
Carbon-rich potassium poly(heptazine imide) for stoichiometric photocatalytic water reduction to hydrogen and glycerol oxidation to high-value products via a direct photocarrier redox pathway 富碳聚七嗪亚胺钾通过直接光载体氧化还原途径,用于化学计量光催化水还原成氢和甘油氧化制高价值产品
IF 9.2 2区 工程技术 Q1 ENERGY & FUELS Pub Date : 2025-12-20 DOI: 10.1016/j.susmat.2025.e01826
Jun-Kai Yeh, Jih-Jen Wu
Carbon-rich potassium poly(heptazine imide) (CKPHI) was synthesized via a direct ionothermal method using a supramolecular complex comprising 2,4,6-triaminopyrimidine (TAP), melamine (MA), and cyanuric acid. Increasing the TAP-to-MA ratio in the precursor promotes substitution of nitrogen atoms in the π-conjugated aromatic framework with carbon atoms and partial conversion of terminal amine groups into cyano and CH moieties, thereby increasing the carbon-to‑nitrogen (C/N) ratio in the resulting CKPHIs. This structural tuning significantly influences light absorption, charge separation, and surface charge transfer behavior, leading to optimized photocatalytic performance of potassium poly(heptazine imide) for simultaneous water reduction and glycerol oxidation. Under AM 1.5G solar illumination (100 mW cm−2) in 10 vol% aqueous glycerol solution, Pt-loaded CKPHI achieves high yields of hydrogen (1648 μmol g−1 h−1), glyceraldehyde (1260 μmol g−1 h−1), dihydroxyacetone (390 μmol g−1 h−1), and cyclic diglycerol (39 μmol g−1 h−1), with glyceraldehyde selectivity reaching 75 %. Moreover, Pt/CKPHI enables stoichiometric hydrogen evolution and selective glycerol oxidation under anaerobic conditions via a direct photocarrier redox pathway, effectively suppressing undesirable CC bond cleavage and overoxidation to carbon dioxide by reactive oxygen species. This work highlights the critical role of structural engineering in ionic carbon nitrides for improving charge dynamics and achieving efficient charge balance in photocatalytic hydrogen generation coupled with biomass valorization.
以2,4,6-三氨基嘧啶(TAP)、三聚氰胺(MA)和三聚氰尿酸为原料,采用直接离子热法制备了富碳聚七嗪亚胺钾(CKPHI)。增加前驱体的tap - ma比,促进π共轭芳骨架中的氮原子被碳原子取代,末端胺基部分转化为氰基和CH基团,从而提高CKPHIs中的碳氮比。这种结构调整显著影响光吸收、电荷分离和表面电荷转移行为,从而优化了聚七嗪亚胺钾同时水还原和甘油氧化的光催化性能。在AM 1.5G太阳光照(100mw cm−2)下,在10 vol%的甘油水溶液中,负载pt的CKPHI获得了高收率的氢(1648 μmol g−1 h−1)、甘油醛(1260 μmol g−1 h−1)、二羟丙酮(390 μmol g−1 h−1)和环甘油(39 μmol g−1 h−1),甘油醛选择性达到75%。此外,Pt/CKPHI可以通过直接光载体氧化还原途径在厌氧条件下进行化学计量析氢和选择性甘油氧化,有效抑制不良的CC键裂解和活性氧对二氧化碳的过度氧化。这项工作强调了结构工程在离子碳氮化物中改善电荷动力学和实现光催化制氢与生物质增值的有效电荷平衡的关键作用。
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引用次数: 0
Optimizing CO2/CH4 selectivity using acid-activated clay for biogas upgrading: A response surface study 酸活性粘土优化沼气升级CO2/CH4选择性:响应面研究
IF 9.2 2区 工程技术 Q1 ENERGY & FUELS Pub Date : 2025-12-19 DOI: 10.1016/j.susmat.2025.e01824
Riya Aneja, Anuj Chauhan, Vipin Kumar Saini
The selective removal of CO2 from biogas is crucial for producing biomethane (Bio-CNG) with higher calorific value and cleaner combustion properties. In this work, acid activation of montmorillonite (MMT) was systematically optimized to enhance its performance as a low-cost, sustainable adsorbent for CO2/CH4 separation. Using a rotatable central composite design (RCCD) within the Response Surface Methodology (RSM) framework, the effects of acid concentration, activation temperature, and treatment time on CO2 adsorption capacity and CO2/CH4 selectivity were investigated. Seventeen acid-activated clay samples (AC − 1 to AC-17) were synthesized, and their adsorption behavior was modeled with the Sips equation. The optimal conditions (acid concentration = 1.9 N, temperature = 28 °C, contact time = 247 min) yielded an optimized acid-activated clay (OAC) with a CO2 uptake of 1.76 mmol·g−1 and a CO2/CH4 selectivity of 121 at 1000 kPa, in close agreement with the predicted value of 118. Structural and textural analysis confirmed significant improvements in surface area (60 to 194 m2·g−1) and pore volume (0.33 to 0.43 cm3·g−1), attributed to dealumination and the formation of silanol groups. Working capacity analysis under PSA (1 bar)/VSA (1 Torr) conditions confirmed the practical separation potential of OAC. These findings demonstrate that optimized acid-activated clays provide a scalable and economical pathway for biogas upgrading, bridging the gap between high-performance synthetic adsorbents and low-cost natural materials.
从沼气中选择性去除二氧化碳对于生产具有更高热值和更清洁燃烧特性的生物甲烷(Bio-CNG)至关重要。本文对蒙脱土(MMT)的酸活化进行了系统优化,以提高其作为低成本、可持续的CO2/CH4分离吸附剂的性能。采用响应面法(RSM)框架下的可旋转中心复合设计(RCCD),研究了酸浓度、活化温度和处理时间对CO2吸附能力和CO2/CH4选择性的影响。合成了17个酸活化粘土样品(AC−1 ~ AC-17),用Sips方程模拟了它们的吸附行为。在酸浓度为1.9 N、温度为28℃、接触时间为247 min的条件下,得到的最佳酸活性粘土(OAC)在1000 kPa下CO2吸收率为1.76 mmol·g−1,CO2/CH4选择性为121,与预测值118基本一致。结构和结构分析证实,由于脱铝和硅醇基团的形成,其表面积(60至194 m2·g−1)和孔隙体积(0.33至0.43 cm3·g−1)有了显著的改善。PSA (1 bar)/VSA (1 Torr)条件下的工作能力分析证实了OAC的实际分离潜力。这些发现表明,优化后的酸活化粘土为沼气升级提供了一条可扩展且经济的途径,弥补了高性能合成吸附剂与低成本天然材料之间的差距。
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Sustainable Materials and Technologies
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