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Techno-economic and life cycle analysis of synthetic natural gas production from low-carbon H2 and point-source or atmospheric CO2 in the United States 美国利用低碳 H2 和点源或大气二氧化碳生产合成天然气的技术经济和生命周期分析
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102791
Kyuha Lee, Pingping Sun, Amgad Elgowainy, Kwang Hoon Baek, Pallavi Bobba

Synthetic natural gas (SNG) is of great interest in reducing fossil energy consumption while maintaining compatibility with existing NG infrastructure and end-use applications equipment. SNG can be produced using clean H2 generated from renewable or nuclear energy and CO2 captured from stationary sources or the atmosphere. In this study, we develop an engineering process model of SNG production using Aspen Plus® and production scales reported by the industry. We examine the levelized cost and life cycle greenhouse gas (GHG) emissions of SNG production under various CO2 supply scenarios. Considering the higher cost of H2 transportation compared with CO2 transportation, we assume that CO2 feedstock is transported via pipeline to the H2 production location, which is collocated with the SNG plant. We also evaluate the cost of CO2 captured from the atmosphere, assuming the direct air capture process can occur near the SNG facility. Depending on the CO2 supply chain, the levelized cost of SNG is estimated to be in the range of $45–76 per million British thermal units (MMBtu) on a higher heating value (HHV) basis. The SNG production cost may be reduced to $27–57/MMBtu-HHV by applying a tax credit available in the United States for low-carbon H2 production (45 V). With a lower electricity price of 3ȼ/kWh for water electrolysis and accounting for a 45 V tax credit, the SNG cost reaches parity with the cost of fossil NG. Depending on the CO2 supply chain, SNG can reduce life cycle GHG emissions by 52–88 % compared with fossil NG.

合成天然气(SNG)在减少化石能源消耗的同时,还能保持与现有 NG 基础设施和终端应用设备的兼容性,因此备受关注。合成天然气可以利用可再生能源或核能产生的清洁 H2 以及从固定来源或大气中捕获的二氧化碳进行生产。在本研究中,我们使用 Aspen Plus® 和行业报告的生产规模开发了 SNG 生产的工程工艺模型。我们研究了各种二氧化碳供应方案下合成天然气生产的平准化成本和生命周期温室气体 (GHG) 排放量。考虑到 H2 运输成本高于 CO2 运输成本,我们假设 CO2 原料通过管道运输到 H2 生产地点,而 H2 生产地点与 SNG 工厂位于同一地点。我们还评估了从大气中捕获二氧化碳的成本,假设直接空气捕获过程可以在合成天然气工厂附近进行。根据二氧化碳供应链的情况,按较高的热值 (HHV) 计算,SNG 的平准化成本估计在每百万英国热量单位 (MMBtu) 45-76 美元之间。如果采用美国为低碳 H2 生产提供的税收减免,SNG 的生产成本可降至 27-57 美元/百万英热单位-HHV(45 V)。如果电解水的电价降低到 3ȼ/kWh 并考虑到 45 V 税收减免,则替代天然气的成本将与化石天然气的成本持平。根据二氧化碳供应链的不同,与化石天然气相比,SNG 可将生命周期内的温室气体排放量减少 52-88%。
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引用次数: 0
Efficient high-throughput screening for the preparation of propylene carbonate in a supercritical microchannel continuous flow system 在超临界微通道连续流系统中高效高通量筛选碳酸丙烯酯的制备方法
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102822
Yan Yang , Xiaotian Liu , Jingfu Jia , Haojia Chen , Xing Mao , Chao Xiong , Hongbing Ji

With the intensification of the global greenhouse effect, the utilization and fixation of CO2 has become one of the most important research fields in our world. However, there are still enormous challenges in achieving efficient fixation and conversion of carbon dioxide into high-value chemicals. Herein, the cycloaddition reaction strategy is adopted to achieve the fixation of supercritical carbon dioxide (SC-CO2) and the high-value conversion of carbon resources to propylene carbonate (PC) by using propylene oxide (PO) as the reaction precursor. Under tetrabutylammonium bromide (TBAB) as a catalyst and water (H2O) as a green solvent, the reaction factors, such as reaction temperature, reaction pressure, catalyst amount, water concentration and molar ratio of reactants, is conducted through the high-throughput screening technology to explore the catalytic performance in a self-designed microchannel reactor. The results indicate that the yield of PC can reach 91.82 % (along with a high selectivity of 99.12 %) at a reaction temperature of 160 ℃, reaction pressure of 8 MPa, catalyst amount of 0.72 mol %, reactants molar ratio of 8, and the residence time of 482 s. Besides, the thermodynamic and kinetic for carbonate synthesis are studied to fully understand the reaction process, and the activation energy of is explored. This work is more efficient than most similar reported works, which provide valuable insights into the practical application of CO2 in the supercritical state combined with microfluidics for synthesizing high-value monomers.

随着全球温室效应的加剧,二氧化碳的利用和固定已成为当今世界最重要的研究领域之一。然而,要实现二氧化碳的高效固定并转化为高价值的化学品仍面临巨大挑战。本文采用环化反应策略,以环氧丙烷(PO)为反应前驱体,实现超临界二氧化碳(SC-CO2)的固定和碳资源向碳酸丙烯酯(PC)的高值转化。在以四丁基溴化铵(TBAB)为催化剂、水(H2O)为绿色溶剂的条件下,通过高通量筛选技术,对反应温度、反应压力、催化剂用量、水浓度和反应物摩尔比等反应因素进行了研究,探讨了在自行设计的微通道反应器中的催化性能。结果表明,在反应温度为 160 ℃、反应压力为 8 MPa、催化剂用量为 0.72 mol %、反应物摩尔比为 8、停留时间为 482 s 的条件下,PC 的产率可达 91.82 %(选择性高达 99.12 %)。此外,还对碳酸盐合成的热力学和动力学进行了研究,以充分了解反应过程,并对活化能进行了探讨。这项工作比大多数类似报告的工作更有效率,为超临界状态下的二氧化碳与微流控技术相结合合成高价值单体的实际应用提供了宝贵的见解。
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引用次数: 0
CO2 conversion to CO by fluidized bed biomass gasification: Measuring CO2 utilization via stable carbon isotope ratios 流化床生物质气化将 CO2 转化为 CO:通过稳定碳同位素比率测量二氧化碳利用率
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102792
Florian Johann Müller , Josef Fuchs , Stefan Müller , Franz Winter

Thermochemical conversion of CO2 in biomass gasification is a promising technology for utilizing CO2 as a feedstock to produce a CO-rich gas. Simultaneous decomposition reactions of biomass and various gas-solid and gas-gas reactions form the product gas in this process. The overlap in sub-processes makes it challenging to assess the conversion of feedstock CO2 with common methods like mass balancing. This work introduces stable carbon isotope ratio analysis (δ13C) to identify the sourcing of carbonaceous product gas components and determine the conversion of CO2. This methodology is applied to evaluate experiments conducted for one hour of continuous operation in a lab-scale fluidized bed gasifier. Softwood pellets and wood char are used as fuel, with Olivine as a bed material, a target heating temperature of 1000 °C and atmospheric pressure. Product gas with more than 80 vol% CO was generated when wood char was used as fuel. Stable carbon isotope measurements show that CO2 is converted at 48–93% in this process, underpinning the position of biomass CO2 gasification as carbon capture and utilization technology. These results were up to 25% higher than suggested by mass balancing, with higher discrepancies at lower CO2 conversions when using softwood as fuel. Therefore, stable carbon isotope ratio measurement can be a valuable tool for improving the process understanding of biomass CO2 gasification. The results can be used for carbon accounting and the technical development of gasifiers with high CO2 utilization efficiency.

在生物质气化过程中进行二氧化碳热化学转化,是利用二氧化碳作为原料生产富含二氧化碳气体的一项前景广阔的技术。在这一过程中,生物质的分解反应和各种气-固、气-气反应同时进行,形成产品气体。由于子过程的重叠,用质量平衡等普通方法评估原料二氧化碳的转化率具有挑战性。这项工作引入了稳定碳同位素比值分析(δ13C),以确定碳质产品气体成分的来源,并确定二氧化碳的转化率。该方法适用于评估在实验室规模的流化床气化炉中连续运行一小时的实验。软木颗粒和木炭用作燃料,床层材料为橄榄石,目标加热温度为 1000 °C,压力为大气压。当使用木炭作为燃料时,生成的气体中 CO 的含量超过 80%。稳定碳同位素测量结果表明,在这一过程中,二氧化碳的转化率为 48-93%,证明了生物质二氧化碳气化技术作为碳捕获和利用技术的地位。这些结果比质量平衡所显示的结果最多高出 25%,当使用软木作为燃料时,二氧化碳转化率较低时,差异会更大。因此,稳定碳同位素比值测量可以作为一种有价值的工具,用于提高对生物质二氧化碳气化过程的认识。测量结果可用于碳核算和具有高二氧化碳利用效率的气化炉的技术开发。
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引用次数: 0
Cycloaddition of limonene epoxide and CO2 over Zn/SBA-15 catalysts for limonene carbonate synthesis 在 Zn/SBA-15 催化剂上进行环氧化柠檬烯和 CO2 的环加成反应以合成碳酸柠檬烯酯
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102817
Carina Mosquera, Aída Luz Villa

The cycloaddition reaction of CO2 with epoxides such as limonene epoxide (LE) to form cyclic carbonates is considered a promising alternative for reducing CO2 emissions. In this work, CO2 fixation on LE to produce cyclic carbonates was carried out over Zn/SBA-15 with tetrabutylammonium bromide (TBAB) as co-catalyst and over NH3X-Zn/SBA-15 (X= Cl, Br, or I) catalysts. The catalysts were characterized by FT-IR, XRD, N2 adsorption–desorption isotherms, TEM, NH3-TPD, XPS, TGA and Py-FTIR. The Zn/SBA-15 support mainly presents Lewis’s acid sites of medium acidity; the surface area was 512 m2/g and 378 m2/g and the pore size were 9 nm and 7.2 nm, for Zn/SBA-15 and NH3Cl-Zn/SBA-15, respectively. The functionalization of Zn/SBA-15 was verified by FTIR, UV-vis, and XPS analysis. It was found that when Zn/SBA-15 was used as catalyst that reaction time had a significative effect on LE conversion and in the case of limonene carbonate selectivity, co-catalyst concentration variation had the main effect. Zn/SBA-15 catalyst can be reused up to 5 times without significant changes neither in conversion nor in limonene carbonate selectivity. The best LE conversion and limonene carbonate selectivity was 33% and 93%, respectively (1 M LE, 200 mg Zn/SBA-15, 7% TBAB; 30 bar, 18 h, 700 rpm and 20 mL diethyl carbonate). The reported catalytic system is a promising system for obtaining limonene carbonate using a heterogeneous catalyst.

二氧化碳与环氧化物(如环氧化柠檬烯(LE))发生环加成反应生成环状碳酸盐被认为是减少二氧化碳排放的一种有前途的替代方法。在这项工作中,以四丁基溴化铵(TBAB)为助催化剂的 Zn/SBA-15 和 NH3X-Zn/SBA-15(X= Cl、Br 或 I)催化剂上进行了二氧化碳固定在 LE 上生成环状碳酸盐的反应。催化剂的表征方法包括傅立叶变换红外光谱、X 射线衍射、N2 吸附-脱附等温线、TEM、NH3-TPD、XPS、TGA 和 Py-傅立叶变换红外光谱。Zn/SBA-15 和 NH3Cl-Zn/SBA-15 的比表面积分别为 512 m2/g 和 378 m2/g,孔径分别为 9 nm 和 7.2 nm。傅立叶变换红外光谱、紫外可见光和 XPS 分析验证了 Zn/SBA-15 的功能化。研究发现,使用 Zn/SBA-15 作为催化剂时,反应时间对 LE 转化率有显著影响,而在柠檬烯碳酸酯选择性方面,助催化剂浓度的变化具有主要影响。Zn/SBA-15 催化剂最多可重复使用 5 次,其转化率和碳酸柠檬烯选择性均无明显变化。最佳的 LE 转化率和柠檬烯碳酸酯选择性分别为 33% 和 93%(1 M LE、200 mg Zn/SBA-15、7% TBAB;30 bar、18 h、700 rpm 和 20 mL 碳酸二乙酯)。所报告的催化系统是一种利用异相催化剂获得碳酸柠檬烯的有前途的系统。
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引用次数: 0
A review of the application of wide-bandgap semiconductor photocatalysts for CO2 reduction 宽带隙半导体光催化剂在二氧化碳还原中的应用综述
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102808
Malathi Arumugam, Hsi-Hsien Yang

Artificial photosynthesis is a viable technique for mitigating the ever-increasing energy demands by converting carbon dioxide (CO2) into energy-rich C1 and C2+ products. A massive contribution to climate change and global warming is the widespread use of fossil fuels, responsible for more than 90% of total CO2 emissions and more than 75% of global greenhouse gas emissions. The most efficient method to convert CO2 into renewable and clean energy is utilizing plentiful sun energy to accelerate photo-induced chemical reactions. Practical CO2 reduction (CO2R), including choosing promising wide-bandgap (WBG) semiconductor photocatalysts with more negative conduction band potential, would be a holy grail for selective fuels and chemicals production. This review article deliberates on the importance of WBG semiconductor photocatalysts and a specific energy level in the conduction band for selective photocatalytic CO2R, which may assist in guiding future photocatalyst design for CO2R. In addition, the summary and prospects of WBG semiconductor photocatalysts and techniques for improving CO2 conversion efficiency and selectivity are discussed.

通过将二氧化碳(CO2)转化为富含能量的 C1 和 C2+ 产物,人工光合作用是缓解日益增长的能源需求的可行技术。化石燃料的广泛使用是造成气候变化和全球变暖的主要原因,其排放量占二氧化碳总排放量的 90% 以上,占全球温室气体排放量的 75% 以上。将二氧化碳转化为可再生清洁能源的最有效方法是利用充足的太阳能来加速光诱导化学反应。切实可行的二氧化碳还原(CO2R),包括选择具有更大负导带电位、前景广阔的宽带隙(WBG)半导体光催化剂,将是选择性燃料和化学品生产的圣杯。这篇综述文章探讨了 WBG 半导体光催化剂的重要性,以及选择性光催化 CO2R 在导带中的特定能级,这可能有助于指导未来 CO2R 光催化剂的设计。此外,文章还讨论了 WBG 半导体光催化剂的总结和前景,以及提高二氧化碳转化效率和选择性的技术。
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引用次数: 0
A bibliometric review on research progress, interest evolution and future trend in the field of recycled concrete by using CiteSpace (2004–2023) 利用 CiteSpace 对再生混凝土领域的研究进展、兴趣演变和未来趋势进行文献计量学审查(2004-2023 年)
IF 7.7 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102826
Li Lin-Bin , Yin Guang-Ji , Wen Xiao-Dong , Miao Ling , Zuo Xiao-Bao , Gao Xiao-Jian

The popularization of recycled concrete (RC) is an important way to achieve efficient resource utilization of construction solid waste (CSW), which can coordinate the sustainable economic development with environmental protection. In this paper, CiteSpace software is used to quantitatively analyze the literatures on RC field, identifying its research hotspots and recent developments. Based on the Web of Science database, we screened published literatures in the field of RC from 2004 to 2023, and obtained 2011 articles. CiteSpace software and knowledge graph technology are adopted to visually analyze the literature information, including the collaborators, keywords and citation status. The results show that, Xiao JZ from Tongji University, Poon CS from Hong Kong Polytechnic University and Tam VWY from University of Western Sydney publish a large number of articles and are frequently cited. It indicates that their researches are widely recognized in academic circles. There is a research team with a large size formed in the Chinese mainland, and the core members include Xiao JZ, Li WG, Chen ZP. At present, the research interest gradually shifts from recycled coarse aggregate to recycled fine aggregate, mainly focusing on microscale research of pore structure and interfacial transition zone. In addition, 8 co-citation clusters of selected references and the potential development trends are detailly analyzed. This study is helpful for researchers to fully understand the current hotspots and future research trends in the field of RC.

推广再生混凝土(RC)是实现建筑固体废弃物(CSW)高效资源化利用的重要途径,可协调经济可持续发展与环境保护的关系。本文利用 CiteSpace 软件对再生混凝土领域的文献进行定量分析,找出其研究热点和最新进展。基于 Web of Science 数据库,我们筛选了 2004 年至 2023 年 RC 领域发表的文献,共获得 2011 篇文章。采用CiteSpace软件和知识图谱技术对文献信息进行可视化分析,包括合作者、关键词和引用情况等。结果表明,同济大学的 Xiao JZ、香港理工大学的 Poon CS 和西悉尼大学的 Tam VWY 发表了大量文章,且被频繁引用。这表明他们的研究得到了学术界的广泛认可。中国大陆也形成了一支规模较大的研究团队,核心成员包括肖 JZ、李 WG、陈 ZP 等。目前,研究兴趣逐渐从再生粗骨料转向再生细骨料,主要集中在孔隙结构和界面过渡带的微观研究。此外,还详细分析了所选参考文献的 8 个共引集群及潜在发展趋势。本研究有助于研究人员全面了解再生骨料领域当前的研究热点和未来的研究趋势。
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引用次数: 0
Fresh, hardened, durability and microstructure properties of seawater concrete: A systematic review 海水混凝土的新鲜、硬化、耐久性和微观结构特性:系统综述
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102815
Abdeliazim Mustafa Mohamed , Bassam A. Tayeh , Samadar S. Majeed , Yazan Issa Abu Aisheh , Musab Nimir Ali Salih

Seawater concrete (SWC) is an environmentally friendly construction material that addresses freshwater scarcity concerns by utilising seawater as a mixing water source. This review study comprehensively examines SWC by focusing on its fresh properties, hardened properties, seawater composition, microstructure and porosity, hydration process, durability, test methods and electrical resistivity. The study analyses the influence of additives and admixtures on SWC’s performance by considering constituents such as cement, aggregates and seawater. It also explores the impact of manufacturing techniques, including mix design. The potential of SWC is revealed and compared with that of conventional concrete by evaluating and comparing their mechanical properties, such as compressive strength, modulus of elasticity, stress-strain behaviours, tensile strength and flexural strength. This study primarily aims to thoroughly examine the characteristics of SWC in its fresh and hardened states. It also assesses the advantages and drawbacks of seawater as a mixing water source. Moreover, this study delves into the impact of seawater composition on crucial aspects, such as the hydration process, microstructure and porosity of concrete. It also used various test methods to explore SWC durability, including resistance to chloride ingress, sulphate attack and carbonation. Furthermore, the importance of electrical resistivity for corrosion prevention is discussed in this study. The carbon-negative cement production and carbonation curing of seawater concrete underscore groundbreaking advancements, emphasizing sustainability and climate mitigation in the construction industry. Overall, this study aims to enhance the comprehension of SWC and provide valuable insights for engineers, researchers and policymakers in concrete technology.

海水混凝土(SWC)是一种环保型建筑材料,它利用海水作为混合水源,解决了淡水稀缺的问题。本综述研究全面考察了海水混凝土的新拌性能、硬化性能、海水成分、微观结构和孔隙率、水化过程、耐久性、测试方法和电阻率。研究通过考虑水泥、集料和海水等成分,分析了添加剂和掺合料对深水泥浆性能的影响。研究还探讨了制造技术(包括混合设计)的影响。通过评估和比较抗压强度、弹性模量、应力-应变行为、抗拉强度和抗折强度等力学性能,揭示了深层螺旋岩混凝土的潜力,并将其与传统混凝土进行比较。本研究的主要目的是深入研究新拌混凝土和硬化混凝土的特性。它还评估了海水作为混合水源的优点和缺点。此外,本研究还深入探讨了海水成分对混凝土水化过程、微观结构和孔隙率等关键方面的影响。研究还采用各种测试方法来探讨海水混凝土的耐久性,包括抗氯化物侵入、硫酸盐侵蚀和碳化的能力。此外,本研究还讨论了电阻率对防腐蚀的重要性。负碳水泥的生产和海水混凝土的碳化养护凸显了突破性进展,强调了建筑行业的可持续性和气候减缓。总之,本研究旨在加深对海水混凝土的理解,并为混凝土技术领域的工程师、研究人员和决策者提供有价值的见解。
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引用次数: 0
Improving the performance of gliding arc plasma-catalytic dry reforming via a new post-plasma tubular catalyst bed 通过新型等离子后管式催化剂床提高滑弧等离子催化干重整的性能
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102820
Wencong Xu , Lukas C. Buelens , Vladimir V. Galvita , Annemie Bogaerts , Vera Meynen

A combination of a gliding arc plasmatron (GAP) reactor and a newly designed tubular catalyst bed (N-bed) was applied to investigate the post-plasma catalytic (PPC) effect for dry reforming of methane (DRM). As comparison, a traditional plasma catalyst bed (T-bed) was also utilized. The post-plasma catalytic effect of a Ni-based mixed oxide (Ni/MO) catalyst with a thermal catalytic performance of 77% CO2 and 86% CH4 conversion at 700 ℃ was studied. Although applying the T-bed had little effect on plasma based CO2 and CH4 conversion, an increase in selectivity to H2 was obtained with a maximum value of 89% at a distance of 2 cm. However, even when only α-Al2O3 packing material was used in the N-bed configuration, compared to the plasma alone and the T-bed, an increase of the CO2 and CH4 conversion from 53% and 53% to 69% and 69% to 83% was achieved. Addition of the Ni/MO catalyst further enhanced the DRM reaction, resulting in conversions of 79% for CO2 and 91% for CH4. Hence, although no insulation nor external heating was applied to the N-bed post plasma, it provides a slightly better conversion than the thermal catalytic performance with the same catalyst, while being fully electrically driven. In addition, an enhanced CO selectivity to 96% was obtained and the energy cost was reduced from ∼ 6 kJ/L (plasma alone) to 4.3 kJ/L. To our knowledge, it is the first time that a post-plasma catalytic system achieves this excellent catalytic performance for DRM without extra external heating or insulation.

研究人员将滑弧等离子体加速器(GAP)反应器和新设计的管式催化剂床(N-bed)相结合,研究了甲烷干转化(DRM)的后等离子体催化(PPC)效应。作为对比,还使用了传统的等离子催化剂床(T-bed)。研究了一种镍基混合氧化物(Ni/MO)催化剂的等离子体后催化效果,该催化剂在 700 ℃ 下的热催化性能为 77% 的 CO2 和 86% 的 CH4 转化率。虽然使用 T 型床对等离子体二氧化碳和甲烷的转化率影响不大,但在距离 2 厘米处,对 H2 的选择性增加,最大值为 89%。不过,即使在 N 型床配置中仅使用 α-Al2O3 填料,与单独使用等离子体和 T 型床相比,CO2 和 CH4 转化率也分别从 53% 和 53% 提高到 69% 和 69% 至 83%。添加 Ni/MO 催化剂进一步增强了 DRM 反应,使 CO2 和 CH4 的转化率分别达到 79% 和 91%。因此,虽然没有对 N-bed 后等离子体进行隔热或外部加热,但在完全电力驱动的情况下,其转化率略高于使用相同催化剂的热催化性能。此外,一氧化碳选择性提高到 96%,能源成本从 6 kJ/L(仅等离子体)降至 4.3 kJ/L。据我们所知,这是首次有一种后等离子体催化系统在没有额外外部加热或隔热的情况下为 DRM 实现如此优异的催化性能。
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引用次数: 0
Influence of morphology and composition of spherical layered double hydroxide particles and derived mixed oxides on photocatalytic CO2 reduction 球形层状双氢氧化物颗粒及其衍生混合氧化物的形态和组成对光催化还原二氧化碳的影响
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102810
Manuel Molina-Muriel , Mahesh Eledath-Changarath , Archit Dhingra , Josep Albero , Juan Francisco Sánchez-Royo , Antonio Ribera , Hermenegildo García

Considering the flexibility in the synthesis that allows the formation of materials with more than two metals, the present study reports the preparation of trimetallic layered double hydroxides (LDHs) having Al as structural tri-positive cation, Ti as photocatalytically active d0 transition metal and either Ni or Co as dipositive cation. In addition, these LDHs were used as precursors of the corresponding trimetallic mixed oxides (MO). LDH and MO materials in combination with Ru(bpy)3Cl2 as photosensitizer and triethanolamine as sacrificial electron donor were used as catalysts for CO2 reduction under solar light irradiation. A different product selectivity, either CH4 for Ni-LDH or CO and H2 for Co-MO, was observed with production rates for CH4 or CO that are among the highest reported for these systems. The role of the inorganic materials in the photocatalytic process was supported by transient absorption spectroscopy that revealed the quenching of the Ru(bpy)3Cl2 triplet excited state by Ni-LDH or Co-MO. An important finding was that the trimetallic Co-Ti-Al oxide with cobaltite structure is able to perform CO2 reduction in spite that the reduction potential of its conduction band is not sufficient to perform the process, evidence by photoluminescence revealing the existence of an upper electronic state responsible for the reduction. These results show the interest in screening multimetallic materials in photocatalysis due to their improved performance and diverse properties.

考虑到合成的灵活性,可以形成含有两种以上金属的材料,本研究报告了三金属层状双氢氧化物(LDHs)的制备方法,其中 Al 为结构性三阳离子,Ti 为光催化活性 d0 过渡金属,Ni 或 Co 为二阳离子。此外,这些 LDHs 还被用作相应的三金属混合氧化物(MO)的前驱体。LDH 和 MO 材料与作为光敏剂的 Ru(bpy)3Cl2 和作为牺牲电子供体的三乙醇胺相结合,被用作催化剂在太阳光照射下还原 CO2。观察到了不同的产物选择性,Ni-LDH 为 CH4,Co-MO 为 CO 和 H2。无机材料在光催化过程中的作用得到了瞬态吸收光谱的支持,该光谱显示了 Ni-LDH 或 Co-MO 对 Ru(bpy)3Cl2 三重激发态的淬灭。一个重要的发现是,具有钴酸盐结构的三金属 Co-Ti-Al 氧化物能够进行二氧化碳还原,尽管其导带的还原电位不足以完成这一过程,光致发光证明存在一个负责还原的上层电子态。这些结果表明,在光催化过程中筛选多金属材料很有意义,因为它们具有更好的性能和多样化的特性。
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引用次数: 0
Novel wastewater recovery process for sustainable sodium carbonate production with CO2 and SOx utilization 利用二氧化碳和硫氧化物可持续生产碳酸钠的新型废水回收工艺
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102824
Jongdu Choi , Jonghun Lim , Yurim Kim , Seongbin Ga , Junghwan Kim

Ammonia-soda process, which produce soda ash, emits flue gas containing a large amount of CO2 and SOx. The wastewater discharged from the ammonia-soda process contains cations, such as Na+ and Ca2+, which can be recovered and reacted with a CO2 and SOx. In this study, we designed a CO2 and SOx utilization process for the sustainable production of sodium carbonate using wastewater recovery system, extracting Na+ and Ca2+. The proposed process involved the following steps: (1) metal-ion separation, which produces NaOH and Ca(OH)2; (2) capture and utilization of SOx using Ca(OH)2; and (3) capture and utilization of CO2 using NaOH and Ca(OH)2, respectively. The economic feasibility of the proposed process was verified by comparing its total annualized cost (TAC) with those of conventional processes. Approximately 99% of SOx was captured to produce high-purity desulfurized gypsum, and 99% of CO2 was captured to be transformed into CaCO3. To confirm the CO2 reduction of the process, the carbon dioxide equivalent (CO2e) was calculated by evaluating the amount of greenhouse gases. The CO2e decreased to 71.4% compared with that of the conventional process. The TAC of the proposed process decreased by 10.67% and 19.63% compared with that of the ammonia-soda and Hou processes, respectively. Thus, this study proposes an industrially potential process design for sustainable sodium carbonate production by utilizing CO2 and SOx with wastewater recycling, without additional reactants, making it more economically viable.

氨碱法生产纯碱,排放的烟气中含有大量二氧化碳和硫氧化物。氨碱法排放的废水中含有 Na+ 和 Ca2+ 等阳离子,这些阳离子可以回收并与 CO2 和 SOx 反应。在这项研究中,我们设计了一种二氧化碳和硫氧化物利用工艺,利用废水回收系统提取 Na+ 和 Ca2+,实现碳酸钠的可持续生产。拟议工艺包括以下步骤:(1) 金属离子分离,产生 NaOH 和 Ca(OH)2;(2) 利用 Ca(OH)2 捕获和利用 SOx;(3) 利用 NaOH 和 Ca(OH)2 分别捕获和利用 CO2。通过比较拟议工艺与传统工艺的总年化成本(TAC),验证了拟议工艺的经济可行性。约 99% 的硫氧化物被捕获,用于生产高纯度脱硫石膏,99% 的 CO2 被捕获,转化为 CaCO3。为了证实该工艺的二氧化碳减排效果,通过评估温室气体的数量计算出了二氧化碳当量(CO2e)。与传统工艺相比,二氧化碳当量减少了 71.4%。与氨-碱工艺和侯工艺相比,拟议工艺的 TAC 分别减少了 10.67% 和 19.63%。因此,本研究提出了一种具有工业潜力的可持续碳酸钠生产工艺设计,通过废水回收利用 CO2 和 SOx,无需额外的反应物,使其更具经济可行性。
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引用次数: 0
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Journal of CO2 Utilization
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