Journal of CO2 Utilization最新文献_第9页

Enhanced plasma-assisted CO2 methanation on Ru/CeO2 catalysts Ru/CeO2催化剂上等离子辅助CO2甲烷化的增强

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-12-01 Epub Date: 2025-10-14 DOI: 10.1016/j.jcou.2025.103240

Beatrice Musig , Jairo Barauna , Abhijit Roy , Raul Arenal , María Elena Gálvez , Tomás García , Ramón Murillo , María Victoria Navarro

Methanation process utilizes CO₂ as a carbon feedstock for synthesizing energy carriers and value-added chemicals. The combination of methanation with plasma-catalysis has emerged as a promising avenue for the electrification of power-to-gas technologies, representing a significant development in the transition to sustainable energy systems. The present study investigates the impact of low 5 % mol Ru loading on CeO₂, focusing in the role of the metal in comparison to Ni and the metal-support interactions examined using CeO₂ with different structures (nanoneedles, nanopowder) and Ru dispersion within the support. The catalyst Ru/NN with nanoneedles of ceria achieved CO₂ conversion of 70 % and CH₄ selectivity of 99 % at 1CO₂/4H₂, WHSV of 30 L h⁻¹ g_cat-1, 12 kg_CO2 kg_cat-1 h⁻¹ and plasma input power of 8.9 W. The enhanced plasma-catalytic activity of Ru/NN can be attributed to the increased effective H₂ dissociation, beneficial physicochemical and electrical properties attributed to the choice of support and optimal metal-support interaction. The lower dielectric capacitance calculated for this catalyst is the result of reduced charge storage and a faster response to the applied electric field. This produces less intense microdischarges and a more stable and uniform plasma environment.

甲烷化过程利用二氧化碳作为碳原料合成能量载体和增值化学品。甲烷化与等离子体催化的结合已成为电力制气技术电气化的一个有前途的途径，代表着向可持续能源系统过渡的重大发展。本研究研究了低5 % mol Ru负载对CeO2的影响，重点研究了金属与Ni的作用，并使用具有不同结构（纳米针、纳米粉末）的CeO2和Ru在载体中的分散来研究金属与载体的相互作用。在1CO₂/4H₂条件下，Ru/NN催化剂的CO₂转化率为70 %，CH₄选择性为99 %，WHSV为30 L h−1 gcat-1, 12 kgCO2 kgcat-1 h−1，等离子体输入功率为8.9 W。Ru/NN的等离子体催化活性增强可归因于有效的H2解离，有利的物理化学和电学性能归因于选择的载体和最佳的金属-载体相互作用。该催化剂的较低介电容量是由于电荷存储减少和对外加电场的更快响应。这会产生较弱的微放电和更稳定和均匀的等离子体环境。

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引用次数: 0

Metal-free conversion of CO2 to non-isocyanate polyurethane for solid amine sorbent pellets design for CO2 capture 无金属二氧化碳转化为非异氰酸酯聚氨酯固体胺吸附剂颗粒设计的二氧化碳捕获

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-12-01 Epub Date: 2025-09-19 DOI: 10.1016/j.jcou.2025.103228

Faranak Heshmatnia, Zahra Eshaghi Gorji, Nguyan Gia Huy, Baljeet Singh, Timo Repo

Green synthesis of non-isocyanate polyurethanes (NIPUs) has attracted considerable interest as an eco-friendly alternative to traditional isocyanate-based routes. In this work, a metal-free catalytic system based on cetyltrimethylammonium bromide (CTAB) was used to transform polyfunctional epoxides into cyclic carbonates with more than 90 % conversion, which can act as key monomer precursors for NIPU formation. Furthermore, the performance of this metal-free catalyst was evaluated in a one-pot process that directly couples epoxides, CO₂ and diamine to yield NIPUs, thereby demonstrating a sustainable strategy for NIPU synthesis that leverages benign catalytic conditions and CO₂ fixation. The synthesized NIPU was explored as a binder to produce shaped solid amine sorbents for CO₂ capture using a 15 % CO₂ stream, with the resulting hollow pellets exhibiting a carbon capture capacity of 29.5 mg/g.

绿色合成非异氰酸酯聚氨酯（nipu）作为传统的基于异氰酸酯的路线的环保替代品引起了相当大的兴趣。本研究利用基于十六烷基三甲基溴化铵（CTAB）的无金属催化体系将多官能团环氧化物转化为环状碳酸盐，转化率超过90% %，可作为NIPU形成的关键单体前体。此外，该无金属催化剂的性能在一锅工艺中进行了评估，该工艺直接将环氧化物，CO 2和二胺偶联产生NIPU，从而证明了利用良性催化条件和CO 2固定来合成NIPU的可持续策略。研究了合成的NIPU作为粘合剂，使用15 % CO2流生产用于CO2捕获的成型固体胺吸附剂，所得中空颗粒的碳捕获能力为29.5 mg/g。

引用次数: 0

Nitrogen-rich covalent triazine frameworks as efficient supports for nickel-catalyzed CO2 conversion 富氮共价三嗪框架作为镍催化CO2转化的有效载体

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-12-01 Epub Date: 2025-11-27 DOI: 10.1016/j.jcou.2025.103279

Mohadeseh Rashvand , Mojtaba Khorasani

A nitrogen-rich covalent triazine framework (CTF) with a low carbon-to-nitrogen (C/N) molar ratio of 1.46 was synthesized as a solid nitrogen-containing ligand, offering abundant coordination sites for the immobilization of nickel(II) acetate catalyst for CO₂ utilization. The resulting heterogeneous Ni-CTF catalyst was thoroughly characterized by porosimetry, TGA, FTIR, Raman spectroscopy, SEM-EDAX, XPS, XRD, and CO₂ adsorption capacity analyses. Ni-CTF efficiently promoted the direct coupling of carbon dioxide with epoxides under relatively mild conditions (0.25 mol% Ni-CTF, 0.5 mol% TBAB, 7.5 bar CO₂, 100 °C). To clarify the individual roles of each catalytic component, a series of control experiments were conducted under identical conditions, including Ni-CTF alone, the pristine CTF, unsupported nickel(II) acetate, and various co-catalysts with distinct chemical properties. These systematic investigations provided deeper insight into the contributions to catalytic performance. Ni-CTF displayed excellent recyclability, retaining both activity and selectivity over at least four consecutive cycles without noticeable loss in performance. The observed catalytic performance is attributed to the organic nature of the CTF, which facilitates the diffusion of organic epoxide molecules, as well as to the nitrogen-rich functionalities embedded within the triazine network. These nitrogen sites, in conjunction with their ability to coordinate nickel species, significantly enhance the CO₂ adsorption capacity of the catalyst.

合成了一种低碳氮（C/N）摩尔比为1.46的富氮共价三嗪框架（CTF）作为固体含氮配体，为固定化乙酸镍催化剂提供了丰富的配位位点。通过孔隙率测定、热重分析、红外光谱、拉曼光谱、SEM-EDAX、XPS、XRD和CO₂吸附量分析对制备的Ni-CTF催化剂进行了全面表征。在相对温和的条件下（0.25 mol% Ni-CTF, 0.5 mol% TBAB, 7.5 bar CO₂，100℃），Ni-CTF能有效促进二氧化碳与环氧化物的直接偶联。为了明确每种催化成分的单独作用，在相同的条件下进行了一系列对照实验，包括单独的Ni-CTF，原始CTF，不负载的醋酸镍（II）和各种具有不同化学性质的助催化剂。这些系统的研究对催化性能的贡献提供了更深入的了解。Ni-CTF表现出优异的可回收性，在至少四个连续循环中保持活性和选择性，而性能没有明显损失。观察到的催化性能归因于CTF的有机性质，它促进了有机环氧化物分子的扩散，以及嵌入在三嗪网络中的富氮功能。这些氮位点，连同它们协调镍种的能力，显著提高了催化剂的CO2吸附能力。

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引用次数: 0

Green and scalable approaches for synthesis and encapsulating clean metal nanoclusters inside cerium MOFs for efficient glycerol carboxylation with CO2 绿色和可扩展的方法合成和封装清洁金属纳米团簇在铈mof内有效的甘油羧化与二氧化碳

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-12-01 Epub Date: 2025-10-17 DOI: 10.1016/j.jcou.2025.103243

Simon Lukato , Agnieszka Krogul-Sobczak , Grzegorz Litwinienko , Ola F. Wendt , Reine Wallenberg , Filip Hallböök , Michal Wojcik

In the pursuit of CO₂-neutral renewable energy solutions, biofuels have emerged as one of the key strategies. However, biodiesel production generates a surplus of crude glycerol (GL), creating a need for efficient valorization pathways. The conversion of GL into value-added chemicals represents a sustainable approach to address this issue. Metal nanoclusters (NCats) embedded within metal-organic frameworks (MOFs) constitute a promising class of hybrid catalysts for GL–CO₂ coupling, yet their controlled synthesis remains limited to a few MOF systems. Herein, we present a clean, scalable, and efficient method for the synthesis of ultra-small, surfactant-free Cu, Ag, and Pd NCats encapsulated in cerium-based MOFs. The resulting catalysts were evaluated in the direct carboxylation of crude GL with CO₂. Among them, the Pd₁Cu₁@MOF1 composite demonstrated outstanding performance, achieving > 73 % yield and a TOF > 100 h⁻¹ with pure GL, and > 14 % yield with a TOF of 30 h⁻¹ using crude GL. The method also enabled successful incorporation of trimetallic PdAgCu NCats, highlighting its potential for the sustainable synthesis of multimetallic NCats-MOF catalytic systems.

在追求二氧化碳中性的可再生能源解决方案的过程中，生物燃料已成为关键战略之一。然而，生物柴油的生产会产生过剩的粗甘油（GL），因此需要有效的增值途径。将GL转化为增值化学品是解决这一问题的可持续方法。嵌入金属有机骨架（MOF）中的金属纳米团簇（NCats）是一类很有前途的GL-CO 2偶联杂化催化剂，但它们的受控合成仍然局限于少数MOF体系。在此，我们提出了一种清洁、可扩展、高效的方法来合成包裹在铈基mof中的超小型、无表面活性剂的Cu、Ag和Pd NCats。对所得催化剂在原油GL与CO₂的直接羧化反应中进行了评价。其中,Pd₁铜₁@MOF1复合显示了卓越的性能,实现祝辞 73 %产量和TOF祝辞 100 h⁻¹ 与纯GL和祝辞 14 %收益率的TOF 30 h⁻¹ 使用原油GL。该方法也使成功整合trimetallic PdAgCu NCats,突出其潜在的可持续的多金属NCats-MOF催化合成系统。

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引用次数: 0

Ion-bridged hydroxyapatite nanofiber bundles via supercritical CO2-mediated mesoscale nanoarchitectonic for robust hydrophobicity 离子桥接羟基磷灰石纳米纤维束通过超临界二氧化碳介导的中尺度纳米结构坚固的疏水性

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-12-01 Epub Date: 2025-10-28 DOI: 10.1016/j.jcou.2025.103263

Wenjing Guo , Yannan Zhou , Binbin Hu , Kanglin Feng , Xuefeng Wei , Shouren Zhang , Baocheng Yang

Conventional hydrophobic ceramic coatings exhibit compromised mechanochemical robustness due to static templating and decoupled organic-inorganic assembly. Here we introduce a supercritical carbon dioxide (SC CO₂) strategy to engineer mesoscale self-assembly—where interactive inorganic-organic building blocks couple across time and space—to enable hierarchical structured hydroxyapatite (HAP) nanofiber bundles with embedded hydrophobicity. Our findings demonstrate that SC CO₂ generates dynamic microcompartments and a mildly acidic environment that not only facilitate the rapid growth of HAP nanofibers with restricted c-axis orientation but also establish directional Ca^2 + –PO₄³⁻ ionic bridges that interconnect nanofibers into a cohesive inorganic network, in which oleate anions (OL⁻) in situ bind at ionic junctions via bidentate chelation, forming a robust hydrophobic layer. This green and scalable process yields advanced hydrophobic ceramic coatings, which have been successfully used to construct HAP-based fire-resistant paper with superior self-cleaning and oil-water separation capability, as well as sustainable Chinese Xuan paper with enhanced writing performance. Such mesoscale engineering, which unifies synthesis, assembly, and function, represents a new paradigm for creating robust, multifunctional biomimetic materials.

传统的疏水陶瓷涂层由于静态模板和去耦的有机-无机组装而表现出较差的机械化学坚固性。在这里，我们介绍了一种超临界二氧化碳（SC CO2）策略来设计中尺度自组装-其中相互作用的无机-有机构建块跨时间和空间耦合-使分层结构羟基磷灰石（HAP）纳米纤维束具有嵌入的疏水性。我们的研究结果表明，SC CO2产生动态微室和温和的酸性环境，不仅促进了具有限制c轴取向的HAP纳米纤维的快速生长，而且还建立了定向Ca2 + -PO43−离子桥，将纳米纤维互连成一个有凝聚力的无机网络，其中油酸阴离子（OL−）通过双牙螯合在离子连接处结合，形成一个坚固的疏水层。这种绿色和可扩展的工艺产生了先进的疏水陶瓷涂层，已成功用于构建具有卓越自清洁和油水分离能力的hap基防火纸，以及具有增强书写性能的可持续中国宣纸。这种中尺度工程将合成、装配和功能结合在一起，代表了一种创造坚固、多功能仿生材料的新范式。

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引用次数: 0

Synthesis of robust S-O covalent-bonded In2S3/α-Fe2O3 nanorod arrays heterojunction with a tailored heat treatment strategy for enhanced photoelectrochemical water splitting 采用定制热处理策略合成S-O共价键In2S3/α-Fe2O3纳米棒阵列异质结，增强光电化学水分解

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-12-01 Epub Date: 2025-10-28 DOI: 10.1016/j.jcou.2025.103260

Ai-zhen Liao , Qing-hua Xie , Lin-ji Zhang , Wei Ren , Yong Wang , Chao Yang , Xiao-hong Jiang , Yong Zhou , Zhi-gang Zou

A robust S-O covalent-bonded In₂S₃/α-Fe₂O₃ nanorod arrays heterojunction were successfully synthesized via a modified heat treatment strategy. The resulting photoanode exhibits an exceptional photocurrent density of 2.65 mA cm⁻² at 1.23 V vs. RHE, achieving a 235 % enhancement compared to robust bare α-Fe₂O₃ (1.13 mA cm⁻² at 1.23 V vs. RHE). To our knowledge, this represents the highest photocurrent density among all reported In₂S₃/α-Fe₂O₃ systems. Moreover, the photoanode demonstrates excellent stability, maintaining over 95 % of its initial performance over 3 h in alkaline electrolyte. The outstanding PEC performances of robust S-O bonded In₂S₃/α-Fe₂O₃ photoanode originates from a synergistic effect of the following aspects: (i) Locking the morphology of FeOOH nanorod array precursor through the improved thermal annealing method decreases charge-carrier recombination; (ⅰi) Forming atomic-level S-O covalent bonds provide direct charge-transfer pathways, thereby enhancing carrier lifetime and reducing interfacial resistance; (iii) Constructing a type-II heterojunction establishes a strong internal electric field that provides a large driving force for the rapid migration of photogenerated charges; and (iv) Loading In₂S₃ efficiently passivates surface defects and promotes hole injection.

通过改进热处理策略，成功合成了一种坚固的S-O共价键In2S3/α-Fe2O3纳米棒阵列异质结。所得到的光阳极在1.23 V vs. RHE下具有2.65 mA cm−2的特殊光电流密度，与α-Fe2O3裸阳极（1.13 mA cm−2,1.23 V vs. RHE）相比，增强了235 %。据我们所知，这代表了所有报道的In2S3/α-Fe2O3体系中最高的光电流密度。此外，光阳极表现出优异的稳定性，在碱性电解质中3 h内保持95% %以上的初始性能。S-O键合In2S3/α-Fe2O3光阳极的优异PEC性能源于以下几个方面的协同效应：(1)通过改进的热退火方法锁定FeOOH纳米棒阵列前驱体的形貌，减少电荷载流子复合；（ⅰ）形成原子级S-O共价键提供了直接的电荷转移途径，从而提高了载流子寿命，降低了界面阻力；（iii）构建ii型异质结建立了强大的内部电场，为光生电荷的快速迁移提供了巨大的驱动力；(4)加载In2S3能有效钝化表面缺陷，促进孔内注入。

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引用次数: 0

Tuning catalyst performance in methane dry reforming via microwave irradiation of Nickel-Silicon carbide systems 微波辐照镍-碳化硅体系对甲烷干重整催化剂性能的调整

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-12-01 Epub Date: 2025-11-05 DOI: 10.1016/j.jcou.2025.103270

Christel Olivier Lenge Mbuya , Kunal Pawar , Mitra Jafari , Parisa Shafiee , Chike George Okoye Chine , Pilar Tarifa , Bogdan Dorneanu , Harvey Arellano-Garcia

The dry reforming of methane (DRM) is a promising route for converting greenhouse gases such as methane (CH₄) and carbon dioxide (CO₂) into valuable syngas, hydrogen (H₂) and carbon monoxide (CO). However, traditional nickel (Ni)-based catalysts suffer from rapid deactivation due to carbon deposition and sintering, especially when supported on low thermal conductivity materials. In this work, a novel post-synthesis microwave irradiation (MIR) treatment is introduced to systematically optimize the performance of Ni – β – SiC and Ni – Ti – Cβ – SiC catalysts for DRM. Unlike previous studies that have used MIR during reaction or with different supports, this approach tunes the metal – support interactions and textural properties of Ni – β – SiC and Ni – Ti – Cβ – SiC catalysts by varying the MIR exposure time after catalyst synthesis. MIR post-treatment (10–25 s) increased the CH₄ conversion to 65 % and the CO₂ conversions to 62 % for Ni–β–SiC catalysts and improved the H₂/CO ratio to 0.80, with stable performance over 20 h. For Ni–Ti–Cβ–SiC, MIR (10–20 s) maintained CH₄ conversion up to 60 % and CO₂ conversion to 58 % over 20 h, while the untreated catalyst, though initially higher, deactivated rapidly. Excessive MIR (30 s) reduced performance for both catalyst types, underscoring the need for optimal exposure time. These findings demonstrate post-synthesis MIR provides a tuneable approach for enhancing both the activity and durability of Ni/SiC – based DRM catalysts through controlled modification of metal – support interactions. This work offers new insights for the design of robust catalysts aimed at greenhouse gas utilization and sustainable syngas production, with activity and stability enhancements linked to controlled changes in metal – support interactions.

甲烷干重整（DRM）是将甲烷（CH4）和二氧化碳（CO2）等温室气体转化为有价值的合成气、氢气（H2）和一氧化碳（CO）的一种有前途的途径。然而，传统的镍基催化剂由于碳沉积和烧结而快速失活，特别是在低导热材料上支撑时。本文介绍了一种新的合成后微波辐照（MIR）处理方法，系统地优化了Ni - β - SiC和Ni - Ti - c - β - SiC催化剂在DRM中的性能。与以往在反应过程中使用MIR或不同载体的研究不同，该方法通过改变催化剂合成后MIR的暴露时间来调节Ni - β - SiC和Ni - Ti - c - β - SiC催化剂的金属-载体相互作用和结构性质。MIR后处理（10-25 s）使Ni -β-SiC催化剂的CH4转化率提高到65 %，CO2转化率提高到62 %，H₂/CO比提高到0.80，在20 H内性能稳定。对于ni - ti - c - β - sic， MIR（10-20 s）在20 h内保持了高达60% %的CH4转化率和58% %的CO2转化率，而未经处理的催化剂虽然最初较高，但很快失活。过多的MIR（30 s）降低了两种催化剂类型的性能，强调了对最佳暴露时间的需求。这些发现表明，合成后的MIR提供了一种可调的方法，通过控制金属载体相互作用的改性来提高Ni/SiC基DRM催化剂的活性和耐久性。这项工作为设计旨在温室气体利用和可持续合成气生产的稳健催化剂提供了新的见解，其活性和稳定性的增强与金属-载体相互作用的可控变化有关。

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引用次数: 0

Application of acid digestion-based total inorganic carbon measurement for carbonated cement-based materials 酸消化法测定总无机碳在碳酸水泥基材料中的应用

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-12-01 Epub Date: 2025-11-05 DOI: 10.1016/j.jcou.2025.103266

Ryo Kurihara , Luge Cheng , Ryusei Igami , Zhenzhen Wang , Abudushalamu Aili , Kiyuki Noto , Minako Tanaka , Haruka Takahashi , Ippei Maruyama

There is growing societal demand for methods to quantify the amount of CO₂ immobilized in cement-based materials. In this study, we compared and evaluated multiple analytical approaches: two different interpretation methods applied to thermogravimetric analysis (TGA) data conventionally used in this field, and two techniques widely adopted in soil science and related areas. The first of these involves heating the sample to release CO₂, which is then quantified using infrared absorption spectroscopy; the second involves dissolving carbonates in the sample using acid, with the evolved CO₂ gas similarly measured using infrared absorption. In carbonated cement pastes, when silica gel and carbonates are in close contact, CO₂ may be released at relatively low temperatures. This temperature range overlaps that of organic matter decomposition, which can complicate quantitative analyses using thermal methods. However, accurate quantification is feasible in systems with minimal organic content. During acid decomposition, silica gel may interfere with carbonate dissolution. Nevertheless, if the sample is sufficiently ground, an appropriate volume of the acid solution is used, and the dissolution time is properly managed under stirring conditions, this method offers a simple and practical means for CO₂ quantification.

社会对量化水泥基材料中固定二氧化碳量的方法的需求越来越大。在这项研究中，我们比较和评估了多种分析方法：两种不同的解释方法应用于该领域的热重分析（TGA）数据，以及两种在土壤科学和相关领域广泛采用的技术。第一种方法是加热样品以释放CO₂，然后使用红外吸收光谱对其进行量化；第二种方法是用酸溶解样品中的碳酸盐，同样用红外吸收法测量释放出的二氧化碳气体。在碳化水泥浆中，当硅胶和碳酸盐紧密接触时，在相对较低的温度下可能会释放CO₂。这个温度范围与有机物分解的温度范围重叠，这会使使用热方法进行定量分析复杂化。然而，在有机含量极低的系统中，精确的定量是可行的。在酸分解过程中，硅胶会干扰碳酸盐的溶解。然而，如果样品充分研磨，使用适当体积的酸溶液，并在搅拌条件下适当管理溶解时间，则该方法为CO₂定量提供了一种简单实用的手段。

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引用次数: 0

Assessment of process conditions in the dry reforming of HDPE fast pyrolysis volatiles for syngas production HDPE快热解挥发物干法重整合成气工艺条件评价

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-12-01 Epub Date: 2025-10-31 DOI: 10.1016/j.jcou.2025.103258

Leire Olazar , Laura Santamaria , Martin Olazar , Maider Amutio , Gartzen Lopez , Maite Artetxe

The joint valorization of CO₂ and high density polyethylene (HDPE) has been carried out by means of a two-stage process consisting of plastic fast pyrolysis and in-line dry reforming. The first step of pyrolysis was carried out in a conical spouted bed reactor (CSBR) by feeding plastics continuously and the volatiles formed were reformed in a second catalytic fluidized bed reactor (FBR), in which Ni commercial methane reforming catalyst has been used. The effect of reforming temperature (600–700 °C), space time (2–25 g_cat min g_HDPE⁻¹) and CO₂/C molar ratio (1−2) on the conversions of HDPE and CO₂ has been analyzed. Furthermore, their influence on the yield of carbon containing products and H₂ production has been analyzed. Thus, an increase in temperature and space time favors HDPE and CO₂ conversion, reaching full HDPE pyrolysis volatiles conversion into gaseous products at temperatures above 650 °C, with a space time of 20 g_cat min g_HDPE⁻¹ and CO₂/C molar ratio of 1.5. Nevertheless, although an increase in CO₂/C molar ratio enhances HDPE conversion, it also leads to CO₂ conversion decrease due to excess CO₂ in the feed. In fact, an increase in all variables above the values corresponding to full conversion of HDPE enhances the reverse Water Gas Shift (WGS) reaction, and therefore increases the conversion of CO₂ to the detriment of H₂ production. Thus, a maximum H₂ production of 0.08 g_H2 g_HDPE⁻¹ has been obtained at 650 °C with a space time of 25 g_cat min g_HDPE⁻¹ and CO₂/C molar ratio of 1.5, attaining a syngas production of 4.7 g_syngas g_HDPE⁻¹.

采用塑料快速热解和在线干重整两段工艺对CO2和高密度聚乙烯（HDPE）进行了联合增值。第一步热解在锥形喷淋床反应器（CSBR）中连续进料进行，挥发分在第二催化流化床反应器（FBR）中进行转化，第二催化流化床反应器采用Ni工业甲烷转化催化剂。分析了重整温度（600 ~ 700℃）、空时（2 ~ 25 gcat min gHDPE−1）和CO2/C摩尔比（1−2）对HDPE和CO2转化的影响。进一步分析了它们对含碳产物收率和H2产率的影响。因此，温度和空间时间的增加有利于HDPE和CO2的转化，在650℃以上的温度下，gHDPE−1的空间时间为20 gcat min， CO2/C摩尔比为1.5，达到HDPE热解挥发物完全转化为气态产物。然而，尽管CO2/C摩尔比的增加提高了HDPE转化率，但由于进料中过量的CO2，也会导致CO2转化率降低。事实上，高于HDPE完全转化对应值的所有变量的增加都增强了反向水气转换（WGS）反应，从而增加了CO2的转化，从而损害了H2的产生。因此，在650°C、25 gcat min gHDPE - 1、CO2/C摩尔比为1.5的条件下，H2的最大产量为0.08 gH2 gHDPE - 1，合成气产量为4.7 gsyngas gHDPE - 1。

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引用次数: 0

Evaporation phase transition dynamic process of liquid CO2 driven by compound heat transfer in storage tanks for mine fire prevention: A theoretical model and experimental studies 矿井防火储罐复合传热驱动液态CO2蒸发相变动力学过程：理论模型与实验研究

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-12-01 Epub Date: 2025-10-29 DOI: 10.1016/j.jcou.2025.103261

Shixing Fan , Yujie Peng , Yankun Ma , Jiarui Zhu , Dengke Wang , Mengru Huang , Wei Wu , Shuo Wu , Zhengdong Liu , Yukun Shi , Jiaxin Ji , Furu Kang , Hu Wen

Mining liquid CO₂ (L-CO₂) storage tanks are vulnerable to external high temperatures and deep geothermal during storage and transportation. The heat is transferred from the outer wall of the storage tank to the interior due to compound heat transfer effects. This ultimately results in the evaporation phase transition of the L-CO₂ inside the tank. The process causes the CO₂ to escape into the air, which increases the risk of asphyxiation in confined spaces for miners and dry ice freeze plugging. Therefore, it is necessary to investigate the evaporation phase transition dynamic process driven by compound heat transfer. In this study, an evaporation phase transition model of L-CO₂ was established based on heat transfer theory and CO₂ phase transition theory. Concurrently, seven types of physical simulation experiments of the evaporation phase transition dynamic process with different schemes were carried out, based on an experimental system for the evaporation phase transition of L-CO₂ that was constructed independently. The influence of ambient temperature and initial filling ratios was considered in the experimental study. On this basis, the relative errors of the theoretical calculation values and experimental data were discussed, and then the accuracy of the evaporation phase transition model was validated. The result indicates that increasing ambient temperature leads to faster rises in temperature and pressure within the L-CO₂ storage tank and extends the evaporation phase transition duration. The initial filling ratio primarily affects the initial storage period. Tanks with a lower initial filling ratio exhibit a more intense evaporation phase transition initially but with a shorter duration. The research results have vital theoretical guiding significance for scientific design and residual quantity prediction of mine L-CO₂ storage tanks.

矿用液态CO2 （L-CO2）储罐在储运过程中容易受到外界高温和深层地热的影响。由于复合传热效应，热量从储罐的外壁传递到内部。这最终导致罐内L-CO2的蒸发相变。这个过程导致二氧化碳逃逸到空气中，这增加了矿工在密闭空间窒息和干冰冻结堵塞的风险。因此，有必要对复合传热驱动下的蒸发相变动力学过程进行研究。本研究基于传热理论和CO2相变理论，建立了L-CO2的蒸发相变模型。同时，在自主构建的L-CO2蒸发相变实验系统的基础上，开展了7类不同方案的蒸发相变动态过程物理模拟实验。实验研究中考虑了环境温度和初始填充率的影响。在此基础上，讨论了理论计算值与实验数据的相对误差，验证了蒸发相变模型的准确性。结果表明：随着环境温度的升高，L-CO2储罐内温度和压力的上升速度加快，蒸发相变时间延长；初始灌装率主要影响初始储存期。初始充注比较低的储罐初始蒸发相变较剧烈，但持续时间较短。研究成果对矿山L-CO2储罐的科学设计和残留量预测具有重要的理论指导意义。

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