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Fixation of high concentration CO2 using Chlorella – Bacteria symbiosis system 利用小球藻-细菌共生系统固定高浓度二氧化碳
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102803
Chuntan Chen , Yu Wang , Qunwei Dai , Weiqi Du , Xinshuang Deng , Yulian Zhao , Qian Duan , Hepei Liu

The mutualistic interaction between microalgae and bacteria provides a new strategy for improving carbon fixation by microalgae. In this study, Chlorella was co-cultured with natural flora at 15 % (v/v) CO2 concentration for 120 d. Three Chlorella symbiotic bacteria strains were identified and were co-cultured with Chlorella vulgaris HL02 (C. vulgaris HL02) to fix high concentrations of CO2. The results showed that the symbiotic bacteria significantly enhanced the fixation of 15 % CO2 by Chlorella, with C. vulgaris HL02 + Aeromonas GS-HL01 having the highest carbon fixation efficiency, which was 22.31 % higher than that of the sterile control, followed by C. vulgaris HL02 + Bacillus GS-F03, and C. vulgaris HL02 + Microbacterium GS-H02 (which was also 16.36 % higher than the sterile control). The composition of harvested Chlorella was not altered significantly following co-culturing with bacteria. Scanning electron microscopy and Excitation–emission matrix spectra analyses showed that at high concentrations of CO2, Microalgae and bacteria promote mutual growth and CO2 fixation mainly through extracellular secretion of organic matter. Our results provided a new strategy to improve the efficiency of microalgae in fixing high concentration of CO2.

微藻类与细菌之间的相互影响为改善微藻类的碳固定提供了一种新策略。在这项研究中,小球藻与天然菌群在二氧化碳浓度为 15% (v/v) 的条件下共培养 120 天。鉴定了三种小球藻共生菌株,并将其与绿球藻 HL02(C. vulgaris HL02)共培养,以固定高浓度的二氧化碳。结果表明,共生菌显著提高了小球藻固定 15% CO2 的能力,其中 C. vulgaris HL02 + 气单胞菌 GS-HL01 的固碳效率最高,比无菌对照高 22.31%,其次是 C. vulgaris HL02 + 芽孢杆菌 GS-F03 和 C. vulgaris HL02 + 微杆菌 GS-H02(也比无菌对照高 16.36%)。与细菌共培养后,收获的小球藻的成分没有明显变化。扫描电子显微镜和激发-发射矩阵光谱分析表明,在高浓度二氧化碳条件下,微藻和细菌主要通过胞外分泌有机物促进相互生长和二氧化碳固定。我们的研究结果为提高微藻固定高浓度二氧化碳的效率提供了一种新策略。
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引用次数: 0
Towards low-cost and sustainable activated carbon production: Influence of microwave activation time on yield and CO2 uptake of PET-derived adsorbents 实现低成本、可持续的活性炭生产:微波活化时间对 PET 衍生吸附剂产量和二氧化碳吸收量的影响
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102807
Emmanuel Dan , Alan J. McCue , Davide Dionisi , Claudia Fernández Martín

Microwave (MW) heating is proposed as a method to transform polyethylene terephthalate (PET) into porous adsorbents. The yield, textural properties, and CO2 uptake of the PET-derived adsorbents irradiated at different durations (3 – 35 min) at 400 °C were assessed. MW activation time influenced both the physical properties and CO2 uptake capacities of the resulting adsorbents. The yield decreased with activation time, but the surface area, total pore volume, micropore volume, and CO2 uptake capacities all increased with MW activation time before declining. The optimal sample (produced with 5 min of MW activation time) showed improved textural properties as well as higher equilibrium and dynamic CO2 uptakes than the commercial activated carbon used as reference. This adsorbent also possesses good selectivity for CO2 in the binary 10:90%vol/vol CO2: N2 mixture. Additionally, an excellent recyclability over 20 cycles, (Regeneration Efficiency > 97%) was observed, and the CO2 adsorption kinetics best fits Lagergren’s pseudo-second-order model. This study has shown that a low activation temperature (400 °C), a short MW activation time (5 min), and a low amount of chemical agent (KOH, 0.72 M) could produce CO2 adsorbents from a cheap and abundant material (PET-waste) with better CO2 uptake to that of a commercial activated carbon.

微波(MW)加热是将聚对苯二甲酸乙二酯(PET)转化为多孔吸附剂的一种方法。评估了在 400 °C 下以不同持续时间(3 - 35 分钟)辐照 PET 衍生吸附剂的产量、质地特性和二氧化碳吸收率。MW活化时间对所得吸附剂的物理性质和二氧化碳吸收能力都有影响。产率随着活化时间的延长而下降,但表面积、总孔体积、微孔体积和二氧化碳吸收能力都随着功率活化时间的延长而增加,然后再下降。与用作参考的商业活性炭相比,最佳样品(用 5 分钟兆瓦活化时间制得)显示出更好的质地特性以及更高的平衡和动态二氧化碳吸收能力。这种吸附剂对 10:90%vol/vol CO2:N2 混合气中对 CO2 具有良好的选择性。此外,经过 20 次循环观察,该活性炭还具有极佳的可回收性(再生效率达 97%),而且二氧化碳吸附动力学最符合拉格伦伪二阶模型。这项研究表明,低活化温度(400 °C)、短 MW 活化时间(5 分钟)和低化学剂用量(KOH,0.72 M)可利用廉价而丰富的材料(PET 废料)生产出二氧化碳吸附剂,其二氧化碳吸附效果优于商业活性炭。
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引用次数: 0
SC-CO2 and emulsion explosives equivalence of rock-breaking effect in granite and mudstone sites SC-CO2 和乳化炸药在花岗岩和泥岩场地的破岩效果等效性
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102806
Nan Jiang , Bin Zhu , Yingkang Yao , Xuedong Luo

How to quantitatively account for the effect of SC-CO2 (Supercritical Carbon) rock-breaking in different rock sites is the key concern in the engineering application of non-explosive rock-breaking technology and economic comparison and there is a lack of experimental basis for relevant studies. Through the equivalent calculation of industrial emulsion explosives, a typical representative granite and mudstone site was selected, and a field experimental program was designed to compare the equivalence of the rock-breaking effects of SC-CO2 and industrial explosives. Based on the rock-breaking equivalent field experiment, we compared and analyzed the rock-breaking area characteristics and parameter changes, such as rock-breaking volume, the morphology of the rock-breaking area, bulk rate, and unit consumption, between SC-CO2 and industrial explosives. A correction of the equivalent conversion formula based on the volume of broken rock was realized. The study shows that SC-CO2 breaks the rock in an elliptical volume shape, the explosives are round, the range of SC-CO2 fracturing breaks the rock is smaller than the range of explosives breaks the rock, and the unit consumption of CO2 is 6–10 times of the unit consumption of explosives. The rock bulk rate is higher after SC-CO2 breaking, while the explosive blast stress wave distribution is uniform, and the bulk rate is low. SC-CO2 rock-breaking produced by the surface vibration velocity is much smaller than the industrial explosives rock-breaking, industrial explosives blasting point of the combined vibration velocity value of the SC-CO2 rock-breaking point of the combined vibration velocity value of 9–11 times, SC-CO2 rock-breaking vibration impact on the surrounding environment is relatively small. The peak combined stress at the measurement point generated by SC-CO2 rock breaking is higher than that of industrial explosives rock breaking, which is 1.2–1.6 times the corresponding measurement point value in the explosives rock breaking test. The study provides an experimental basis for research on the equivalence of SC-CO2 rock-breaking and industrial explosives rock-breaking.

如何定量核算SC-CO2(超临界碳)在不同岩场的破岩效果,是非爆破破岩技术工程应用和经济对比的关键问题,相关研究缺乏实验依据。通过对工业乳化炸药的等效计算,选取了具有代表性的典型花岗岩和泥岩场地,设计了现场实验方案,比较了 SC-CO2 和工业炸药的破岩效果等效性。在破岩等效现场实验的基础上,对比分析了 SC-CO2 和工业炸药的破岩面积特征和参数变化,如破岩量、破岩面积形态、散装率和单耗等。实现了基于破岩体积的等效换算公式的修正。研究表明,SC-CO2 破岩体积呈椭圆形,而炸药呈圆形,SC-CO2 压裂破岩范围小于炸药破岩范围,二氧化碳单耗是炸药单耗的 6-10 倍。SC-CO2 破岩后岩石松散率较高,而炸药爆破应力波分布均匀,松散率较低。SC-CO2破岩产生的地表振动速度远小于工业炸药破岩,工业炸药爆破点的综合振动速度值是SC-CO2破岩点综合振动速度值的9-11倍,SC-CO2破岩振动对周围环境影响相对较小。SC-CO2破岩产生的测点综合应力峰值高于工业炸药破岩,是炸药破岩试验相应测点值的1.2-1.6倍。该研究为研究 SC-CO2 破岩与工业炸药破岩的等效性提供了实验依据。
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引用次数: 0
Benchmarking microwave-induced CO2 plasma splitting against electrochemical CO2 reduction for a comparison of promising technologies 将微波诱导的二氧化碳等离子体分裂与电化学二氧化碳还原作为基准,以比较有前途的技术
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102825
A. Hecimovic , M.T. Mayer , L.G.J. de Haart , S. Gupta , C.K. Kiefer , A. Navarrete , A. Schulz , U. Fantz

Plasma conversion technology is an emerging technique under development to activate, convert or valorize gas molecules such as CO2, N2, CH4, NH3 and others. A large-scale application beyond the lab-scale demonstrator unit requires assessment of the efficiency of this new technology. The straightforward approach for assessment of the efficiency is benchmarking with the other well-established technologies of similar technology readiness level (TRL). In this paper we present a benchmarking of the atmospheric pressure microwave-induced CO2 plasma splitting with electrochemical CO2 conversion, via both low-temperature and high-temperature electrolysis. An additional step of oxygen removal in case of the plasma reactor is implemented due to the difference in the output stream of the plasma (gas mixture containing CO2, CO, and O2) and the electrochemical reactor (typical gas mixture on cathode containing CO2 and CO). For the benchmarking, a comprehensive set of comparison parameters that are applicable for both the plasma and the electrochemical route is identified and grouped in three comparison categories: performance, interfaces, and economics. The comparison of these parameters demonstrates that in terms of the electric power consumption (EPC; power required for production of one Nm3CO) plasma conversion technology (∼20 kWh/Nm3CO) is in the ballpark with the other two electrochemical technologies (∼4–20 kWh/Nm3CO). The key features of the plasma conversion technology are relatively large conversion (up to 56%) and moderate energy efficiencies (up to 27%). Also, CO2 gas of reduced purity of only 98% can be used without decrease of the performance, and CO output values are currently at 3.5 slm (standard litre per minute). Fast on/off response time of order of minutes, and no need for the hot standby indicate that the plasma conversion is particularly suitable for use of intermittent renewable energy sources. The aspects that require further development include optimization of the process towards lower EPCtotal values, improved oxygen gas separation, and reliable ignition of the plasma.

等离子体转换技术是一种正在开发的新兴技术,用于激活、转换或提升 CO2、N2、CH4、NH3 等气体分子的价值。要在实验室规模的示范装置之外进行大规模应用,就必须对这一新技术的效率进行评估。评估效率的直接方法是与技术就绪水平(TRL)类似的其他成熟技术进行基准比较。在本文中,我们介绍了通过低温和高温电解进行常压微波诱导二氧化碳等离子体分裂与电化学二氧化碳转换的基准。由于等离子体(含有 CO2、CO 和 O2 的混合气体)和电化学反应器(阴极上含有 CO2 和 CO 的典型混合气体)的输出流不同,因此在等离子体反应器中增加了除氧步骤。为进行基准比较,确定了一套适用于等离子体和电化学路线的综合比较参数,并将其分为三个比较类别:性能、界面和经济性。这些参数的比较表明,在电能消耗(EPC;生产一 Nm3CO 所需的电能)方面,等离子体转换技术(∼20 kWh/Nm3CO)与其他两种电化学技术(∼4-20 kWh/Nm3CO)相差无几。等离子转换技术的主要特点是转换率相对较高(高达 56%),能效适中(高达 27%)。此外,使用纯度仅为 98% 的二氧化碳气体也不会降低性能,目前二氧化碳的输出值为 3.5 slm(标准升/分钟)。几分钟的快速开关响应时间和无需热备用表明,等离子体转换特别适合使用间歇性可再生能源。需要进一步开发的方面包括优化工艺以降低 EPCtotal 值、改进氧气分离和等离子体的可靠点火。
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引用次数: 0
Microwave thermal pre-treatment and calcination of biomineralised sorbents for calcium looping 微波热预处理和煅烧用于钙循环的生物矿化吸附剂
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102794
María Erans , Gabriela Durán-Jimenez , José M. Rodríguez , Lee Stevens , Chris Dodds

Waste eggshells have been investigated as biomineralised CO2 sorbents for the calcium looping cycle due to their high Ca content, low cost, availability, and high CO2 uptake. This work investigates a novel heat-pre-treatment using eggshells as raw material. The eggshells were simultaneously calcined and thermally pre-treated via microwave heating using different powers and times whilst maintaining the same input energy in a single mode cavity reactor. The calcined eggshells were characterised using standard characterisation techniques such as TGA and isotherms of N2 adsorption at 77 K. The dielectric properties were measured using the cavity perturbation technique at 2.45 GHz. Numerical electromagnetic simulations were performed using COMSOL Multiphysics and results were used to optimise the experimental setup. The treated materials were subjected to carbonation/calcination cycles in order to assess their suitability as a calcium-looping sorbent. The sorbent that exhibited a more stable CO2 uptake was the one treated at the highest power (800 W) 4.5 mmol CO2/g sorbent after 20 cycles under mild calcination conditions. Adsorbents prepared at 400, 600 and 800 W displayed similar CO2 uptake after 20 cycles when the calcination conditions were under more realistic conditions.

废弃蛋壳因其钙含量高、成本低、可用性强和二氧化碳吸收率高,已被研究用作钙循环的生物矿化二氧化碳吸附剂。这项工作研究了一种以蛋壳为原料的新型热预处理方法。在单模空腔反应器中,使用不同的功率和时间,同时保持相同的输入能量,通过微波加热同时对蛋壳进行煅烧和热预处理。煅烧后的蛋壳采用标准表征技术进行表征,如 TGA 和 77 K 下的 N2 吸附等温线。在 2.45 GHz 频率下使用空腔扰动技术测量了介电性能。使用 COMSOL Multiphysics 进行了数值电磁模拟,并将模拟结果用于优化实验装置。对处理过的材料进行了碳化/煅烧循环,以评估其作为钙循环吸附剂的适用性。在温和的煅烧条件下,以最高功率(800 瓦)处理的吸附剂在 20 个循环后的二氧化碳吸收率为 4.5 mmol CO2/g。当煅烧条件更为实际时,用 400、600 和 800 W 制备的吸附剂在 20 个循环后显示出相似的二氧化碳吸收率。
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引用次数: 0
Value-added recycling of waste concrete fines into alternative aggregates for river sand conservation 将废弃混凝土细料回收增值为河沙保护的替代骨料
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102802
Renjie Zhou , Yunjie Luo , Mingfang Ba , Zihua Zhang , Jianghua Fang , Chi Sun Poon , Xiaoliang Fang

Due to the depletion of river sand, the construction industry is eager to develop upcycling techniques for transforming secondary by-products derived from construction and demolition (C&D) waste into quality fine aggregates. This paper presents a study of replacing river sand with enhanced recycled fine aggregate through a wet carbonation process developed by the authors previously. The fine recycled concrete aggregate (FRCA) ranging from 0.15 to 5 mm was prepared by demolishing a concrete with a known mixture design. After wet carbonation, the particle size, water absorption, and density of the FRCA were tested and compared with the original samples. The chemical characteristics of the original and carbonated FRCA (C-FRCA) were analyzed by a series of experiments. The results showed that (1) an increase of carbonation products and a significant reduction of hydration products; (2) microscopic observation of the C-FRCA showed a surface layer densified by calcite after wet carbonation; and (3) no significant strength loss were observed when replacing up to 50% river sand by C-FRCA in mortar specimens. The potential environmental and economic impacts were also analyzed.

由于河砂的枯竭,建筑行业迫切希望开发升级再循环技术,将建筑和拆除(C&D)废料中的次级副产品转化为优质细骨料。本文介绍了一项通过作者之前开发的湿碳化工艺,用强化再生细骨料替代河砂的研究。0.15 至 5 毫米的细再生混凝土骨料(FRCA)是通过已知混合物设计的混凝土拆卸制备的。湿法碳化后,对 FRCA 的粒度、吸水性和密度进行了测试,并与原始样品进行了比较。通过一系列实验,分析了原始和碳化后 FRCA(C-FRCA)的化学特性。结果表明:(1) 碳化产物增加,水化产物显著减少;(2) C-FRCA 的显微镜观察显示,湿碳化后方解石使表面层致密化;(3) 在砂浆试样中用 C-FRCA 替代 50% 的河砂时,未观察到明显的强度损失。此外,还分析了潜在的环境和经济影响。
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引用次数: 0
Carbon dioxide sequestration in cementitious materials: A review of techniques, material performance, and environmental impact 水泥基材料中的二氧化碳封存:技术、材料性能和环境影响综述
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102812
Omer Ahmed , Shamsad Ahmad , Saheed K. Adekunle

The release of carbon dioxide (CO2) into the earth's atmosphere is a substantial global environmental concern that arises from the processes of industrialization and urbanization. The increase in atmospheric CO2 concentrations has resulted in the phenomenon of global warming and subsequent alterations in climate patterns. Accelerated CO2 sequestration in cementitious materials is currently the subject of extensive research as a highly efficacious approach to mitigating the carbon footprint of the concrete industry. The sequestration procedure entails the transformation of gaseous CO2 into carbonate minerals. The review presented in this paper outlines the most recent carbonation (i.e., CO2 sequestration) techniques, such as mineral carbonation, accelerated CO2 curing (ACC), pre-carbonation, and carbonation mixing, that have been recently explored. The potential of mineral carbonation of industrial wastes and the advantages of their incorporation in the concrete matrix is investigated. Carbonation technologies and their effect on the performance of cementitious composites are reported. Information on life cycle assessment are also included to evaluate the environmental impact associated with the production of carbonated materials. Various commercialized CO2 utilization technologies in construction sector, such as CarbonCure, Solidia, Carbstone, Calera, and Carbon8 are reviewed. Moreover, this review offers a thorough insight into the carbonation technologies, evaluating their advantages, limitations, and the existing gaps in research.

二氧化碳(CO2)释放到地球大气中是工业化和城市化过程中产生的一个重大全球环境问题。大气中二氧化碳浓度的增加导致了全球变暖现象以及随之而来的气候模式的改变。加速水泥基材料中的二氧化碳封存是目前广泛研究的主题,是减轻混凝土行业碳足迹的一种高效方法。封存过程需要将气态二氧化碳转化为碳酸盐矿物。本文概述了最近探索的最新碳化(即二氧化碳封存)技术,如矿物碳化、二氧化碳加速固化(ACC)、预碳化和碳化混合。本文研究了工业废料矿物碳化的潜力以及将其掺入混凝土基质的优势。报告了碳化技术及其对水泥基复合材料性能的影响。还包括生命周期评估信息,以评估与碳化材料生产相关的环境影响。综述了建筑行业中各种商业化的二氧化碳利用技术,如 CarbonCure、Solidia、Carbstone、Calera 和 Carbon8。此外,本综述还深入分析了碳化技术,评估了其优势、局限性以及现有的研究空白。
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引用次数: 0
Simultaneous enhancement of CO2 adsorption capacity and kinetics on a novel micro-mesoporous MIL-101(Cr)-based composite: Experimental and DFT study 新型微多孔 MIL-101(Cr)基复合材料同时增强二氧化碳吸附容量和动力学:实验和 DFT 研究
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102809
Mohammad Bazmi , Alimorad Rashidi , Abbas Naderifar , Farnaz Tabarkhoon , Masood S. Alivand , Farnoush Tabarkhoon , Mehran Vashaghani Farahani , Mehdi D. Esrafili

MIL-101(Cr), a class of metal-organic framework, is a potential candidate for CO2 capture applications because of its high capacity of adsorption and separation capability. However, the intrinsic microporous structure of this nanomaterial poses limitations on its adsorption kinetics. Techniques employed to enhance its adsorption kinetics often adversely impact its adsorption capacity at equilibrium. Herein, as a new approach, we prepared amine-functionalized FAC@MIL-101(Cr) composites with adjustable micro-mesoporous structure and tunable nitrogen content by embedding different ratios of amine-functionalized activated carbon throughout the framework of MIL-101(Cr). This led to a simultaneous improvement in both kinetics and adsorption capacity for CO2. The best adsorbent, FAC-6@MIL-101(Cr), has excellent textural properties with a high surface area (1763.1 m2.g−1), great pore volume (1.29 cm3.g−1), and suitable nitrogen content (4.7 wt%). The adsorption analysis revealed that the modification of MIL-101(Cr) improved its CO2 adsorption capacity from 3.21 to 5.27 mmol/g under standard conditions of 1 bar and 25 °C. Furthermore, the FAC-6@MIL-101(Cr) adsorbent demonstrated fast CO2 adsorption kinetics (three times more relative to the pure MIL-101(Cr)), high CO2/N2 selectivity, and remarkable cyclic stability. The results confirmed that hybridization enhanced the polarizability of FAC@MIL-101(Cr) samples, causing more robust CO2-adsorbent surface interactions. Simultaneously, the existence of mesopores in the structure facilitated the transport of CO2 into the interior pores, resulting in a more efficient contact of CO2 molecules with all of the amine sites and a faster adsorption rate as well as more efficient regeneration. According to density functional theory (DFT) calculations, hybridization process induces significant changes in composites’ electronic structure, enhancing their capacity to interact with CO2 molecules more effectively. On the other hand, DFT calculations confirm that N2 molecule is less activated on the FAC@MIL-101(Cr) as evidenced by calculated small adsorption energy and charge-transfer values.

MIL-101(Cr)是一类金属有机框架,具有很强的吸附能力和分离能力,是二氧化碳捕集应用的潜在候选材料。然而,这种纳米材料固有的微孔结构限制了其吸附动力学。为提高其吸附动力学而采用的技术往往会对其平衡吸附能力产生不利影响。在此,作为一种新方法,我们通过在整个 MIL-101(Cr) 框架中嵌入不同比例的胺功能化活性炭,制备了具有可调微孔结构和可调氮含量的胺功能化 FAC@MIL-101(Cr)复合材料。这同时提高了动力学性能和对二氧化碳的吸附能力。最佳吸附剂 FAC-6@MIL-101(Cr)具有优异的质地特性,比表面积高(1763.1 m2.g-1),孔隙率大(1.29 cm3.g-1),氮含量合适(4.7 wt%)。吸附分析表明,在 1 bar 和 25 °C 的标准条件下,对 MIL-101(Cr)的改性将其二氧化碳吸附容量从 3.21 mmol/g 提高到了 5.27 mmol/g。此外,FAC-6@MIL-101(Cr) 吸附剂表现出快速的二氧化碳吸附动力学(是纯 MIL-101(Cr) 的三倍)、高 CO2/N2 选择性和显著的循环稳定性。结果证实,杂化增强了 FAC@MIL-101(Cr)样品的极化性,使 CO2-吸附剂表面的相互作用更强。同时,中孔结构的存在促进了 CO2 向内部孔隙的传输,使 CO2 分子与所有胺位点更有效地接触,吸附速率更快,再生效率更高。根据密度泛函理论(DFT)计算,杂化过程会导致复合材料的电子结构发生显著变化,从而增强其与二氧化碳分子更有效地相互作用的能力。另一方面,密度泛函理论计算证实,N2 分子在 FAC@MIL-101(Cr)上的活化程度较低,这一点可以从计算出的较小吸附能和电荷转移值得到证明。
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引用次数: 0
Biocatalytic cofactor regeneration for CO2 reduction: Integration of a hydrogenase and a formate dehydrogenase in H2-driven systems 二氧化碳还原的生物催化辅助因子再生:氢气驱动系统中氢化酶和甲酸脱氢酶的整合
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102828
Michael Groh , Elisabeth Lettau , Janna Schoknecht , Jan Liedtke , Lars Lauterbach , Silke Leimkühler

Formate dehydrogenases catalyze the reversible oxidation of formate to carbon dioxide. These enzymes play an important role in CO2 reduction and serve as nicotinamide cofactor recycling enzymes. More recently, the CO2-reducing activity of formate dehydrogenases, especially metal-containing formate dehydrogenases, has been further explored for efficient atmospheric CO2 capture. In this sense, molecular hydrogen (H2) as the fuel of the future represents an efficient, cheap and environmentally friendly reducing agent when produced from renewable sources. Hydrogenases are enzymes that catalyze the reversible oxidation of H2. Herein, the functional interplay between the soluble [NiFe] hydrogenase from Cupriavidus necator and the molybdenum-dependent formate dehydrogenase from Rhodobacter capsulatus was investigated in a coupled biocatalytic system. H2-driven CO2 reduction (H2CO2R) using methyl viologen as an artificial electron mediator gave a higher product yield of formate than using NAD+ as the physiological electron mediator. The enzymes were stable under anaerobic conditions for 18 h, making the coupled reaction suitable for biotechnological purposes.

甲酸脱氢酶催化甲酸盐可逆地氧化成二氧化碳。这些酶在二氧化碳还原过程中发挥着重要作用,同时也是烟酰胺辅助因子循环酶。最近,人们进一步探索了甲酸脱氢酶(尤其是含金属的甲酸脱氢酶)的二氧化碳还原活性,以高效捕获大气中的二氧化碳。从这个意义上说,分子氢(H2)作为未来的燃料,从可再生资源中生产出来,是一种高效、廉价和环保的还原剂。氢化酶是催化 H2 可逆氧化的酶。在此,我们在一个耦合生物催化系统中研究了来自坏死葡萄球菌(Cupriavidus necator)的可溶性[NiFe]氢酶和来自荚膜罗杆菌(Rhodobacter capsulatus)的依赖钼的甲酸脱氢酶之间的功能相互作用。与使用 NAD+ 作为生理电子介质相比,使用甲基紫精作为人工电子介质的 H2 驱动 CO2 还原(H2CO2R)可获得更高的甲酸产物产量。这些酶在厌氧条件下可稳定工作 18 小时,使耦合反应适用于生物技术目的。
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引用次数: 0
Exploring the role of surface and porosity in CO2 capture by CaO-based adsorbents through response surface methodology (RSM) and artificial neural networks (ANN) 通过响应面法(RSM)和人工神经网络(ANN)探索表面和孔隙率在氧化钙基吸附剂捕获二氧化碳过程中的作用
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102773
Enrique Martínez de Salazar Martínez , María F. Alexandre-Franco , Alberto J. Nieto-Sánchez , Eduardo M. Cuerda-Correa

In this study, synthetic CaCO3 materials were utilized as precursors for CaO-based CO2 sorbents. The investigation examined how various operating parameters—such as synthesis temperature (ST), stirring rate (SR), and surfactant percentage (SP)—impact the properties of the adsorbents. Samples were firstly characterized by X-ray diffraction and Scanning Electron Microscopy (SEM), which revealed that the prevalence of calcite or aragonite crystal phases in the synthetic CaCO3 precursors can be tuned by adequately choosing the dose of surfactant (Triton-X100®), so that it can be used as a crystal habit and growth modifier. The calcination process applied to the CaCO3 precursors leads to the formation of partially sinterized cubic crystals of CaO, accompanied by minor quantities (< 5 %) of additional compounds like Ca(OH)2 or CaSO4. Specific surface area (SBET) and porosity were determined by measuring the N2 adsorption isotherms. A CaCO3 sample with an unprecedented value of SBET as large as 116 m2/g was prepared operating under optimal conditions. SBET and pore volumes were successfully correlated with the CO2 uptake capacity of the samples. SBET is more influential for experiments carried out under diluted CO2 atmosphere. When pure CO2 is used, the influence of meso- and micropore volumes (Vme and Vmi) is clearly predominant, which suggests that in this latter case diffusion through the porous texture of the samples plays a more remarkable role. A double-way approach through Response Surface Methodology (RSM) and the use of Artificial Neural Networks (ANNs) has been used to analyze the CO2 uptake capacity of the samples. Within the operational interval, excellent results were obtained for pure and diluted CO2 flow, and RSM and ANNs have demonstrated to be a very efficient tool to correlate the behavior of the CaO-based materials as CO2 sorbents with the surface area and pore volumes of the samples. Valuable information on (i) the importance of the different factors under study; (ii) their influence on the surface and porosity of the CaO-derived sorbents; and (iii) the subsequent CO2 capture performance of the sorbents has been obtained. The results suggest that four parameters have a statistically significant influence on CO2 uptake. These parameters are SR, the square of SR, its interaction with SP, and the square of SP. Additionally, the study assessed the stability of the CaO-based sorbents over 11 consecutive calcination-carbonation cycles. By adequately choosing the synthesis strategy and conditions, an almost negligible shrinkage effect can be achieved, resulting in a more sustained uptake capacity throughout the cycles.

本研究利用合成 CaCO3 材料作为 CaO 基二氧化碳吸附剂的前体。研究考察了各种操作参数(如合成温度 (ST)、搅拌速率 (SR) 和表面活性剂百分比 (SP))对吸附剂特性的影响。首先利用 X 射线衍射和扫描电子显微镜 (SEM) 对样品进行表征,结果表明,通过适当选择表面活性剂(Triton-X100®)的剂量,可以调整合成 CaCO3 前体中方解石或文石晶体相的普遍性,从而使其成为晶体习性和生长调节剂。煅烧 CaCO3 前驱体的过程会形成部分烧结的立方体 CaO 晶体,并伴有少量(< 5 %)Ca(OH)2 或 CaSO4 等其他化合物。比表面积 (SBET) 和孔隙率是通过测量 N2 吸附等温线确定的。在最佳条件下制备的 CaCO3 样品的 SBET 值达到了前所未有的 116 m2/g。SBET 和孔隙体积成功地与样品的二氧化碳吸收能力相关联。SBET 对在稀释的 CO2 大气中进行的实验影响更大。当使用纯二氧化碳时,中孔和微孔体积(Vme 和 Vmi)的影响明显占主导地位,这表明在后一种情况下,通过样品多孔质地的扩散起着更加显著的作用。通过响应面法(RSM)和人工神经网络(ANN)双管齐下,对样品的二氧化碳吸收能力进行了分析。在运行区间内,纯二氧化碳流和稀释二氧化碳流都获得了优异的结果,RSM 和 ANNs 被证明是一种非常有效的工具,可将氧化钙基材料作为二氧化碳吸附剂的行为与样品的表面积和孔隙体积相关联。在以下方面获得了宝贵的信息:(i) 所研究的不同因素的重要性;(ii) 它们对 CaO 衍生吸附剂表面和孔隙率的影响;以及 (iii) 吸附剂随后的二氧化碳捕获性能。结果表明,有四个参数对二氧化碳的吸收有显著的统计学影响。这些参数是 SR、SR 的平方、SR 与 SP 的相互作用以及 SP 的平方。此外,研究还评估了 CaO 基吸附剂在连续 11 次煅烧-碳化循环中的稳定性。通过适当选择合成策略和条件,几乎可以忽略收缩效应,从而在整个循环过程中获得更持久的吸收能力。
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引用次数: 0
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Journal of CO2 Utilization
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