Journal of CO2 Utilization最新文献_第2页

CO2 and steam-CO2 reforming of ethanol over CuО/Al2O3 catalysts: Influence of additives on catalyst coking 乙醇在CuО/Al2O3催化剂上的CO2和蒸汽-CO2重整：添加剂对催化剂焦化的影响

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2026-01-20 DOI: 10.1016/j.jcou.2026.103333

Gaukhar Yergaziyeva , Moldir Anissova , Nursaya Makayeva , Laura Myltykbayeva , Manshuk Mambetova , Zhengisbek Kuspanov , Chingis Daulbayev , Madina Bissenova

The effect of γ-Al₂O₃ modification with CeO₂ and La₂O₃ oxides on the catalytic and performance characteristics of copper catalysts in CO₂ reforming and steam–CO₂ reforming of ethanol is investigated. Catalysts with compositions of 10 wt% CuO/Al₂O₃, 10 wt% CuO/2 wt% CeO₂–Al₂O₃ and 10 wt% CuO/2 wt% La₂O₃–Al₂O₃ were synthesized, characterized by TPD-CO₂, TPR-H₂, TPO, TGA/DTA and XRD techniques, and tested in the temperature range of 500–800 °C. The addition of La₂O₃ was shown to generate the strongest basic sites and suppress the formation of the CuAl₂O₄ spinel phase, resulting in an optimal combination of high CO₂ conversion (95 %), maximum hydrogen concentration (55.3 vol%), and minimal coking under steam–CO₂ reforming conditions. In contrast, CeO₂ addition enhances oxygen mobility and promotes ethanol dehydration activity but leads to the highest ethylene yield (67.5 vol%) and the greatest coke deposition (167 mgC/gcat), particularly in the presence of steam. A linear correlation (R² ≈ 0.98) between ethylene yield and the amount of deposited carbon was identified, indicating the key role of ethylene as a coke precursor in the investigated systems. Thermogravimetric analysis of spent catalysts revealed that the La-modified catalyst accumulated the lowest amount of predominantly reactive carbon species and exhibited the lowest deactivation rate. The obtained results establish the relationship between basicity, redox properties, and coking tendency in CuO/Al₂O₃–CeO₂/La₂O₃ systems, providing a rational basis for the design of stable copper catalysts for ethanol reforming with simultaneous CO₂ utilization.

研究了用ceo2和La₂O₃氧化物改性γ-Al₂O₃对铜催化剂在乙醇CO₂重整和蒸汽- CO₂重整过程中的催化性能和性能的影响。合成了10 wt% CuO/Al₂O₃、10 wt% CuO/2 wt% CeO₂-Al₂O₃和10 wt% CuO/2 wt% La₂O₃-Al₂O₃的催化剂，采用TPD-CO₂、TPR-H₂、TPO、TGA/DTA和XRD技术对催化剂进行了表征，并在500 ~ 800℃的温度范围内进行了测试。结果表明，在蒸汽- CO₂重整条件下，La₂O₃的加入产生了最强的碱性位点，抑制了CuAl₂O₄尖晶石相的形成，从而实现了高CO₂转化率（95% %）、最大氢浓度（55.3 vol%）和最小结焦的最佳组合。相比之下，添加CeO 2可以提高氧的流动性，促进乙醇脱水活性，但导致最高的乙烯收率（67.5 vol%）和最大的焦炭沉积（167 mgC/gcat），特别是在有蒸汽存在的情况下。乙烯产率与沉积碳量呈线性相关（R²≈0.98），表明乙烯作为焦炭前驱体在研究体系中起着关键作用。对废催化剂的热重分析表明，la改性催化剂的主要活性碳含量最低，失活率最低。所得结果建立了CuO/Al₂O₃-CeO₂/La₂O₃体系的碱度、氧化还原性能和结焦倾向之间的关系，为设计稳定的铜催化剂用于乙醇重整同时利用CO₂提供了合理的依据。

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引用次数: 0

Study on enhancing natural gas recovery by CO2 injection in water-bearing heterogeneous carbonate reservoirs 含水非均质碳酸盐岩储层注CO2提高天然气采收率研究

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2026-01-19 DOI: 10.1016/j.jcou.2026.103332

Shiwen Ji , Youcheng Zheng , Youquan Liu , Ruoyu Yang , Yan Zhang , Yuehan Wei

The technology of switching to CO₂ in natural gas reservoirs to enhance natural gas recovery is highly recognized for its ability to store carbon dioxide and improve gas recovery rates. However, the application of this technology in carbonate reservoirs with edge and bottom water presents two main challenges: the significant heterogeneity of carbonate rocks and the pronounced intrusion of edge and bottom water. This study investigates the mechanisms of Enhanced Gas Recovery and the basic laws of gas-water seepage in reservoirs through laboratory physical simulation experiments. Using core samples with varying permeability, high and low permeability conditions were simulated to characterize the heterogeneity of carbonate reservoirs. The experimental results indicate that: 1. After switching to CO₂, high-permeability cores have better energy replenishment effects compared to low-permeability cores, with the recovery rate of high-permeability cores improving by 8.2 % compared to low-permeability cores; 2. The injected carbon dioxide can effectively push back the formation water that has intruded into both high and low permeability cores, releasing natural gas that was previously trapped by the formation water, thus alleviating the adverse effects of water intrusion that lead to low recovery rates; 3. Under different injection pressures, the recovery degree of high-permeability cores is consistently higher than that of low-permeability cores; when the pressure recovers to 100 %, the recovery rate of high-permeability cores reaches its highest level at 76.97 %, which is 30.79 % higher than that of low-permeability cores. Therefore, CO₂-EGR technology demonstrates significant potential in controlling water intrusion and improving recovery efficiency in carbonate gas reservoirs.

天然气储层转换为CO2以提高天然气采收率的技术因其储存二氧化碳和提高天然气采收率的能力而受到高度认可。然而，在具有边底水的碳酸盐岩储层中，该技术的应用面临着两大挑战：碳酸盐岩非均质性明显，边底水侵入明显。通过室内物理模拟实验，探讨了提高采收率的机理和储层气水渗流的基本规律。利用不同渗透率的岩心样品，模拟了高、低渗透条件下碳酸盐岩储层的非均质性特征。实验结果表明：1。转换成CO2后，高渗透岩心的能量补充效果优于低渗透岩心，高渗透岩心的采收率比低渗透岩心提高了8.2 %；2. 注入的二氧化碳可以有效地将侵入高渗透和低渗透岩心的地层水推回，释放出之前被地层水困住的天然气，从而缓解水侵入导致采收率低的不利影响；3. 在不同注入压力下，高渗透岩心的采收率始终高于低渗透岩心；当压力恢复到100 %时，高渗透岩心的采收率最高，为76.97 %，比低渗透岩心的采收率高30.79 %。因此，CO2-EGR技术在控制碳酸盐岩气藏水侵、提高采收率方面具有很大的潜力。

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引用次数: 0

Coupling DRM and NO reduction: A catalyst design strategy to control coking in Ni-based catalysts 耦合DRM和NO还原：一种控制镍基催化剂焦化的催化剂设计策略

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2026-01-17 DOI: 10.1016/j.jcou.2026.103313

Beatrice Senoner , Andrea Osti , Davide Chinello , Giovanni Agostini , Antonella Glisenti

In the scenario of climate change, dry reforming of methane (DRM) is a well-studied reaction where CO₂ and CH₄ are converted into syngas, a mixture composed of CO and H₂ widely used in industries. However, DRM industrialization is hindered by the high operating temperatures and catalyst deactivation, mainly due to coking - i.e., carbon deposition. This work aims to mitigate the coking problem by alternating DRM with a NO flux which gasifies carbon above 677 °C into CO/CO₂. Three Ni-impregnated catalysts are designed for this dual process: the chosen supports are γ-Al₂O₃, for its high dispersion and strong interaction with Ni, LaFeO₃, for its NOx abatement properties and a mixed support LaFeO₃-Al₂O₃. Only by combining the support properties in Ni/LaFeO₃-Al₂O₃ catalyst nickel particles can be protected by NO oxidation, allowing increased conversions after NO flux and highlighting the need of combining catalyst and process design to achieve efficient and synergical pollutants abatement.

在气候变化的情景下，甲烷干重整（DRM）是一个被充分研究的反应，其中CO2和CH4转化为合成气，这是一种由CO和H2组成的混合物，广泛用于工业。然而，DRM工业化受到高温和催化剂失活的阻碍，主要是由于焦化-即碳沉积。这项工作旨在通过将DRM与NO熔剂交替使用，将677°C以上的碳气化成CO/CO2，从而缓解焦化问题。为此设计了三种镍浸渍催化剂：选择的载体是γ-Al2O3，因为它具有高分散性和与Ni的强相互作用，LaFeO3，因为它具有减少NOx的性能，以及混合载体LaFeO3- al2o3。只有结合Ni/LaFeO3-Al2O3催化剂中的支撑性能，镍颗粒才能受到NO氧化的保护，从而增加NO通量后的转化率，并突出了催化剂和工艺设计相结合的必要性，以实现高效和协同的污染物减排。

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引用次数: 0

Preparation of high purity CaCO3 by carbonation of carbide slag after physical impurity removal: calcination, cyclone and magnetic separation 电石渣经煅烧、旋流器、磁选等物理除杂后碳化制备高纯碳酸钙

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2026-01-17 DOI: 10.1016/j.jcou.2026.103329

Zhuohui Ma , Wenhao Ning , Huaigang Cheng , Bo Wang

The co-production of high-purity CaCO₃ by carbonating CO₂ from carbide slag (CS) has attracted significant attention. However, due to the complex composition of CS and the difficulty in separating Ca element, it is difficult to balance the carbonation cost and quality of the product. In this study, CS was used as raw material, and a method of preparing high-purity CaCO₃ through calcination, cyclone and magnetic separation, named multi-stage impurity removal, was proposed firstly. The effects of calcination time and temperature on mineral phase transformation and the purity and whiteness of CaCO₃ prepared by carbonation during the calcination of carbide slag were studied. The effects of cyclone and magnetic separations were also discussed. The mechanism for the removal of impurities through high-temperature calcination was discussed innovatively. The optimum process conditions for multi-stage impurity removal and carbonation were determined, after calcination at 900 ℃ for 3 h, the CS was transported to cyclone separation at an inlet volumetric flow rate of 80 m³ /h. The separated substrate was then formulated into a pulp with a S/L of 10 % for magnetic separation. The CS pulp obtained after magnetic separation entered the carbonation process, where it was aerated with CO₂ at a flow rate of 0.2 L/min for carbonation. This process resulted in calcite-type CaCO₃ with the purity and whiteness of 97.8 % and 97.4, respectively. Finally, the cost of the process was estimated. The total initial investment cost was approximately CNY 6.51 million, while the total operating cost was CNY 1915.85/t of CaCO₃.

利用电石渣（CS）碳化CO2联产高纯碳酸钙已引起广泛关注。但由于CS成分复杂，且Ca元素难以分离，难以平衡碳酸化成本和产品质量。本研究以CS为原料，首次提出了一种煅烧-旋风-磁选制备高纯CaCO3的多级除杂方法。研究了煅烧时间和煅烧温度对电石渣煅烧过程中矿物相变及碳化法制备CaCO3纯度和白度的影响。讨论了旋流分离和磁选的影响。创新性地探讨了高温煅烧脱除杂质的机理。确定了多级除杂碳化的最佳工艺条件，经900℃煅烧3 h后，以80 m³ /h的进口体积流量将CS输送到旋风分离器中分离。然后将分离的底物配制成S/L为10 %的纸浆进行磁选。磁选后得到的CS矿浆进入碳酸化过程，以0.2 L/min的流速充入CO2进行碳酸化。该工艺可制得纯度为97.8% %、白度为97.4%的方解石型CaCO3。最后，对该工艺的成本进行了估算。初始投资总成本约651万元，运行总成本为1915.85元/t CaCO3。

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引用次数: 0

Silica-supported nickel catalysts synthesized via the molten salt method for reverse water-gas shift: Impact of chlorine and bromine halides 熔融盐法合成二氧化硅负载镍催化剂用于逆水气转换：氯和卤化溴的影响

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2026-01-16 DOI: 10.1016/j.jcou.2026.103330

Jia-Ying Sie , Tzu-Hung Wen , Po-Yang Peng , Ying-Rui Lu , Chi-Liang Chen , Yu-Chuan Lin

Nickel catalysts supported on silica were synthesized via a molten salt method (MSM) using Na- and K-based salts with Cl⁻ or Br⁻ counterions, and evaluated in low-temperature reverse water–gas shift (RWGS) reaction. Despite similar Ni nanoparticle sizes, the presence of residual salts significantly influenced catalyst performance by altering the electronic properties of Ni and the nature of surface carbonates. X-ray absorption spectroscopy (XAS) revealed negatively charged Ni species (Ni^δ⁻), particularly in Br-containing samples. H₂-temperature programmed reduction (TPR) and X-ray photoelectron spectroscopy (XPS) confirmed Ni-Cl and Ni-Br interactions, and the latter showed a higher extent. In-situ infrared studies indicated that Br-based catalysts suppressed the formation of bidentate carbonate (b-*CO₃), a spectator that passivates active sites, and instead favored monodentate carbonate (m-*CO₃), leading to higher CO₂ conversions. The r-Ni@Na_1.9K_3.3Br(5)/SiO₂ catalyst achieved stable CO₂ conversion (ca. 35 %) with 100 % CO selectivity and 100-hour durability. These results highlight the importance of halide identity in modulating Ni–salt interactions and reaction pathways for RWGS.

采用熔融盐法（MSM）合成了二氧化硅负载镍催化剂，并在低温逆水气变换（RWGS）反应中进行了评价。尽管镍纳米颗粒大小相似，但残余盐的存在通过改变镍的电子性质和表面碳酸盐的性质而显著影响催化剂的性能。x射线吸收光谱（XAS）发现带负电荷的Ni （Niδ⁻），特别是在含br的样品中。h2 -温度程序还原（TPR）和x射线光电子能谱（XPS）证实了Ni-Cl和Ni-Br的相互作用，后者表现出更高的程度。原位红外研究表明，br基催化剂抑制了双齿碳酸盐（b-*CO3）的形成，而有利于单齿碳酸盐（m-*CO3）的形成，从而导致更高的CO2转化率。r-Ni@Na1.9K3.3Br(5)/SiO2催化剂实现了稳定的CO2转化率（约35 %），CO选择性为100% %，耐久性为100小时。这些结果强调了卤化物身份在调节镍盐相互作用和RWGS反应途径中的重要性。

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引用次数: 0

Molybdenum and tungsten carbides as catalysts for the reverse water gas shift reaction 碳化钼和碳化钨作为水煤气倒转反应的催化剂

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2026-01-16 DOI: 10.1016/j.jcou.2026.103327

Dahi Akmach , Shang Jiang , Anik Ashirwadam , Malak El Kaddouri , Samir H. Mushrif , Serge Kaliaguine , David S.A. Simakov

For the sustainable utilization of carbon dioxide (CO₂), the development of an inexpensive, active, selective and highly stable catalyst is essential to overcome the economic challenges in its reduction to carbon monoxide (CO). Molybdenum and tungsten carbides-based materials are regarded as attractive catalysts for the reverse water gas shift RWGS reaction. This work began with a series of catalytic tests indicating that mixed Mo-W carbides behave essentially like blends of monocarbides Mo₂C and WC. To establish a performance baseline, an in-depth evaluation of the two monometallic carbides was conducted enabling a precise assessment of their intrinsic activity and mechanistic behavior under RWGS conditions. The results revealed that Mo₂C promoted the formation of both CH₄ and CO, while increasing the tungsten content gradually, enhances CO selectivity with decreasing reaction rate. Monometallic tungsten carbide WC achieved complete CO selectivity and maintained it even after 100 h exposure to harsh reaction conditions at 600 ˚C. In-situ DRIFTS and density functional theory (DFT) calculations revealed that WC can achieve 100 % CO selectivity through two distinct mechanisms on different facets, a concerted redox mechanism on WC (-100), and an associative mechanism on WC (101) facet where further hydrogenation of *CHO intermediate is kinetically unfavorable. Both pathways steer the reaction toward CO production and prevent the formation of undesired side product CH₄. This work not only provides valuable insights into the role of metal carbide phases in catalytic performance but also contributes to the fundamental understanding of reaction mechanism.

为了可持续利用二氧化碳（CO2），开发一种廉价、活性、选择性和高度稳定的催化剂对于克服将其还原为一氧化碳（CO）的经济挑战至关重要。碳化钨钼基材料被认为是水煤气倒转RWGS反应的理想催化剂。这项工作从一系列的催化测试开始，表明混合的Mo-W碳化物的行为基本上就像Mo2C和WC的单碳化物的混合物。为了建立性能基准，研究人员对这两种单金属碳化物进行了深入评估，从而精确评估了它们在RWGS条件下的内在活性和机制行为。结果表明，Mo2C对CH4和CO的生成均有促进作用，而随着反应速率的降低，钨的含量逐渐增加，CO的选择性增强。单金属碳化钨WC具有完全的CO选择性，即使在600˚C的恶劣反应条件下暴露100 h后也能保持这种选择性。原位漂移和密度泛函理论（DFT）计算表明，WC可以通过两种不同面的机制实现100% %的CO选择性，即WC（-100）面的协同氧化还原机制和WC（101）面的结合机制，其中*CHO中间体的进一步加氢在动力学上是不利的。这两种途径都将反应导向CO的产生，并防止不需要的副产物CH4的形成。这项工作不仅对金属碳化物相在催化性能中的作用提供了有价值的见解，而且有助于对反应机理的基本理解。

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引用次数: 0

Ultra-rapid direct dissociation of CO₂ with dense pulsed plasma jets for Martian oxygen production 用密集脉冲等离子体射流超快速直接解离二氧化碳，用于火星氧气生产

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2026-01-15 DOI: 10.1016/j.jcou.2026.103326

Adrian Scurtu, Dorina Ticoş, Constantin Diplaşu, Nicoleta Udrea, Maria Luiza Mitu, Beatrice Paraschiv, Cătălin M. Ticoş

Intense pulsed plasma jets with electron densities of in excess of 10²¹ m⁻³ and temperatures of ∼13 eV were used to dissociate CO₂ under Martian pressure conditions at 1–5 Torr for in-situ oxygen production. Our method demonstrated 20–50 times greater temporal efficiency than an RF plasma, which achieved a 23 % conversion in ∼450 s. This advantage stems from our method’s reduced sensitivity to non-thermal back reactions and thermal recombination, as well as its notably short CO₂ dissociation time of just 5 nanoseconds. A peak conversion rate of 33.29 % was reached at 1 Torr, with an O₂ produced mass of 5.5 mg per pulse at 5 Torr. Energy efficiency reached 7.2 % at a low specific energy input (SEI) of less than < 11 eV/molecule, surpassing RF and DC plasmas which feature 1.6 %, although all plasma systems exhibit reduced efficiency at low pressures due to high SEI from low molecular density. These findings highlight pulsed plasma jets as a promising, scalable solution for rapid oxygen generation on Mars, with optimization via larger chambers and possibly catalysts approach.

利用电子密度超过10²¹ m⁻³ 和温度为~ 13 eV的强脉冲等离子体射流，在1-5 Torr的火星压力条件下解离CO₂，用于原位制氧。我们的方法证明了比射频等离子体高20-50 倍的时间效率，在~ 450 秒内实现了23 %的转换。这一优势源于我们的方法降低了对非热反反应和热复合的敏感性，以及它的CO₂解离时间非常短，仅为5纳秒。在1 Torr时，转化率达到33.29 %，在5 Torr时，每脉冲产生的O₂质量为5.5 mg。在低于 11 eV/分子的低比能输入（SEI）下，能量效率达到了7.2 %，超过了RF和DC等离子体的1.6 %，尽管所有等离子体系统在低压下由于低分子密度的高SEI而降低了效率。这些发现强调了脉冲等离子体射流作为一种有前途的、可扩展的解决方案，可以通过更大的腔室和可能的催化剂方法进行优化，在火星上快速生成氧气。

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引用次数: 0

Nanofluidic replication of reservoir pore networks on silicon chips: New insights of the miscibility of CO2–alkane systems in nano-confined spaces 硅芯片上储层孔隙网络的纳米流体复制：纳米密闭空间中co2 -烷烃体系混相的新见解

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2026-01-15 DOI: 10.1016/j.jcou.2026.103324

Xiuxiu Pan , Linghui Sun , Huiwen Xiao , Qingjie Liu , Zhirong Zhang , Xu Huo , Yuhan Wang , Feiyu Chen , Boyu Jiang

The supercritical properties of CO₂ and its carbon neutrality properties drive its wide application in geological utilization and storage, but the complex structural characteristics of reservoir nanopores restrict the utilization of CO₂. In this study, we innovatively integrate molten wood’s metal perfusion technology and the formation nanopore reproduction process, constructing a nanosilicon-based chip (characteristic scales: 1μm, 200 nm, 100 nm, 30 nm) based on the topological characteristics of the pore network of shale reservoirs.We systematically reveal the dynamic miscibility behavior of CO₂ and seven alkane components (C₆-C₁₂) within confined space. The experimental results indicate that the nanoconfinement effect significantly reduces the minimum miscible pressure (MMP) of the system, with the maximum reduction reaching 4.18 % at 30 nm (0.68 % and 2.56 % at 200 nm and 100 nm, respectively). The miscible component intervals are also scale-dependent and can be classified into three characteristic regions based on MMP: below C₆ (fast miscible zone), C₇-C₁₁ (transitional miscible zone), and above C₁₂ (hysteresis miscible zone). Furthermore, for the first time, the component differentiation phenomenon of mixed alkane systems was understood in homogeneous and heterogeneous fracture-pore systems. We propose a coupled approach of "digital replication of reservoir pores and in-situ nanofluidic observation" to reproduce the miscible process between CO₂ and key components of crude oil. This novel method, along with robust experimental data, is expected to serve as a valuable reference for the further development of CO₂ geological utilization.

CO2的超临界特性及其碳中性特性推动了其在地质利用和封存中的广泛应用，但储层纳米孔复杂的结构特征限制了CO2的利用。本研究创新性地将熔融木的金属灌注技术与地层纳米孔再生过程相结合，根据页岩储层孔隙网络的拓扑特征，构建了特征尺度为1μm、200 nm、100 nm、30 nm的纳米硅基芯片。我们系统地揭示了CO2与七种烷烃组分（C6-C12）在密闭空间内的动态混相行为。实验结果表明，纳米约束效应显著降低了体系的最小混相压力（MMP），在30 nm处最大降低了4.18 %，在200 nm和100 nm处分别降低了0.68 %和2.56 %。混相成分层段也具有尺度依赖性，根据MMP可划分为C6以下（快速混相带）、C7-C11（过渡混相带）和C12以上（滞后混相带）三个特征区。首次在均质和非均质缝孔体系中认识了混合烷烃体系的组分分异现象。提出了一种“储层孔隙数字复制与纳米流体原位观察”的耦合方法来再现CO2与原油关键组分的混相过程。这种新方法以及可靠的实验数据有望为进一步发展二氧化碳地质利用提供有价值的参考。

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引用次数: 0

Emerging 2D–Ti3C2Tx-MXene nanomaterial anchored on MIL-101(Cr) metal-organic framework as solid adsorbent for CO₂ capture under ambient conditions 新型2D-Ti3C2Tx-MXene纳米材料锚定在MIL-101（Cr）金属有机骨架上作为固体吸附剂在环境条件下捕获CO₂

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2026-01-13 DOI: 10.1016/j.jcou.2026.103322

Sehrish Shoukat , Jaeseok Heo , Jungmin Yang , Duckshin Park

The increasing accumulation of CO₂ in the atmosphere has intensified the need for efficient carbon dioxide capture materials. However, it is a challenge to come up with an optimum solid CO₂ adsorbent that can substitute chemical adsorption for large-scale applications. Among various solid sorbents, metal-organic frameworks (MOFs) combined with newly emerging two-dimensional (2D) nanomaterials, Ti₃C₂T_x-MXene, have attracted significant attention owing to their higher porosity, tunable structures, and large surface areas and physisorption mechanism. In this study, we describe the utilization of 2D Ti₃C₂T_x-MXene anchored on MIL-101(Cr) MOF in solid form to evaluate their CO₂ adsorption performance using a fixed-bed adsorption column. Advanced characterization of the as-produced adsorbent is conducted using XRD, FTIR, SEM with EDS, TGA, and BET analysis to assess their surface morphology, surface groups, chemical composition, and surface properties. The synthesized composite showed a BET surface area of 2138 m²/g and a pore volume of ∼1.34 cm³/g. In the adsorption column, CO₂ breakthrough measurements were performed by a continuous CO₂ concentration (15 %) with an inlet flow of 40 mL/min at 1 atm and 25 °C. The CO₂ adsorption capacity (∼21 mg/g) was achieved by Ti₃C₂T_x-MXene/MIL-101 (Cr) at ambient conditions. This corresponds to ∼50 % better performance than pristine MIL-101 (Cr) at similar conditions. Moreover, the Ti₃C₂T_x-MXene/MIL-101 (Cr) offers good regeneration performance with no significant loss in CO₂ adsorption capacity in regenerative cycles. Finally, the novel work with good CO₂ adsorption results opens a new window of implications of emerging nanomaterials as a promising material platform for CO₂ capture applications for further investigation under direct air capture conditions (ultra-low CO₂ concentrations).

大气中二氧化碳的积累日益增加，加强了对有效的二氧化碳捕获材料的需求。然而，如何找到一种可以代替化学吸附大规模应用的最佳固体CO2吸附剂是一个挑战。在各种固体吸附剂中，金属有机骨架（MOFs）与新兴的二维（2D）纳米材料Ti3C2Tx-MXene相结合，因其孔隙率高、结构可调、比表面积大、吸附机理好而备受关注。在这项研究中，我们描述了利用固定床吸附柱，以固体形式固定在MIL-101(Cr) MOF上的2D Ti3C2Tx-MXene，来评估它们对CO2的吸附性能。利用XRD、FTIR、SEM、EDS、TGA和BET分析对所制备的吸附剂进行了深入表征，以评估其表面形貌、表面基团、化学成分和表面性能。合成的复合材料的BET比表面积为2138 m2/g，孔体积为~ 1.34 cm3/g。在吸附柱中，CO2突破测量采用连续CO2浓度（15 %），进口流量为40 mL/min，温度为1 atm，温度为25℃。在环境条件下，Ti3C2Tx-MXene/MIL-101 （Cr）的CO2吸附量为~ 21 mg/g。这相当于在类似条件下比原始MIL-101 （Cr）的性能提高~ 50 %。此外，Ti3C2Tx-MXene/MIL-101 （Cr）具有良好的再生性能，在再生循环中没有明显的CO2吸附能力损失。最后，这项具有良好二氧化碳吸附效果的新工作为新兴纳米材料的应用打开了一扇新的窗口，纳米材料作为一种有前途的材料平台，可以在直接空气捕获条件下（超低二氧化碳浓度）进一步研究二氧化碳捕获应用。

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引用次数: 0

Growth of ionic polymers on ZIFs to construct core-shell hybrid materials via coordination interactions for catalytic CO₂ conversion 离子聚合物在zif上生长，通过配位作用构建核壳杂化材料，催化CO₂转化

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2026-01-13 DOI: 10.1016/j.jcou.2026.103325

Jinquan Wang , Xiukai Li , Siew Ping Teong , Shook Pui Chan , Zibiao Li , Xinglong Zhang , Yugen Zhang

A sustainable and practical method has been developed for synthesizing ZIF-ionic polymer core-shell hybrid materials. This one-pot, two-step process employs imidazole, zinc nitrate, DABCO (1,4-diazabicyclo[2.2.2]octane), and 1,3,5-tris(bromomethyl)benzene in ethanol, yielding high efficiency. In this approach, DABCO facilitates ZIF formation by deprotonating imidazole and subsequently reacts with 1,3,5-tris(bromomethyl)benzene to generate a poly-DABCO salt that coats the ZIF surface via coordination interactions. The resulting hybrid materials, which exhibit dual Lewis acid and base functionalities, demonstrate exceptional activity and stability in catalyzing CO₂ conversion into cyclic carbonates. Interestingly, the catalyst also exhibits high activity in the synthesis of bis(cyclic carbonate) from diepoxide, which subsequently reacts with diamines to form non-isocyanate polyurethanes. A proposed reaction mechanism, combining experimental findings and density functional theory (DFT) calculations, highlights the critical roles of zinc and the ionic polymer in achieving high catalytic performance. Specifically, zinc and ionic polymer are identified as key contributors to epoxide activation and ring-opening processes. This study not only deepens the understanding of ZIF-polymer hybrid materials but also establishes a strong foundation for future advancements in their design, research, and applications.

开发了一种可持续实用的合成zif离子聚合物核壳杂化材料的方法。该工艺采用咪唑、硝酸锌、DABCO（1,4-重氮杂环[2.2.2]辛烷）和1,3,5-三（溴乙基）苯为原料，一锅两步制得效率高。在这种方法中，DABCO通过去质子化咪唑促进ZIF的形成，随后与1,3,5-三（溴乙基）苯反应生成聚DABCO盐，通过配位作用覆盖在ZIF表面。所得到的杂化材料具有双重刘易斯酸和碱功能，在催化二氧化碳转化为环状碳酸盐方面表现出优异的活性和稳定性。有趣的是，该催化剂在二氧化物合成双（环碳酸酯）中也表现出高活性，随后与二胺反应形成非异氰酸酯聚氨酯。结合实验结果和密度泛函理论（DFT）计算，提出了一种反应机制，强调了锌和离子聚合物在实现高催化性能方面的关键作用。具体来说，锌和离子聚合物被认为是环氧化物活化和开环过程的关键因素。这项研究不仅加深了对zif -聚合物杂化材料的理解，而且为其未来的设计、研究和应用奠定了坚实的基础。

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引用次数: 0