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Revealing the structure-activity relationship of Mn3O4/TiO2 via phase engineering for enhanced photocatalytic CO₂ reduction 通过相工程揭示Mn3O4/TiO2增强光催化CO 2还原的构效关系
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-02-16 DOI: 10.1016/j.jcou.2026.103357
Eunhee Gong , Hye Rim Kim , Yunju Hwang , Jeonghyeon Lee , Jin-Woo Jung , Chang-Hee Cho , In Young Kim , Su-Il In
The structure-activity relationship plays a crucial role for enhanced photocatalytic performance, nevertheless, precisely controlling the phase of transition metal oxides remains a significant challenge. Herein, we developed 2D-layered Mn3O4 decorated with TiO2 catalyst to investigate the effects of manganese oxide phase on photocatalytic CO2 reduction activity. We optimized the manganese oxide phase by varying the amount of the TiCl4 precursor. During the synthesis reaction, TiCl4 is a key role for determining the oxidation state of manganese oxide. We identified that Mn3O4 is the best phase for photocatalytic CO2 reduction, and Mn3O4/TiO2 exhibits 20.1-, 7.8-fold enhanced photocatalytic CO2 reduction performance than pristine TiO2 and Mn3O4, respectively. The improved photocatalytic activity is relevant to the phase of manganese oxide, the enhanced separation of charge carriers and prolonged lifetimes of charge carriers. In situ X-ray Absorption Near-Edge Structure (XANES) confirms the changes of oxidation state under photocatalytic CO2 reduction conditions. Furthermore, the photocatalytic mechanism is proposed by in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis. This study provides an effective design strategy for modulating oxidation state of transition metal oxide-based photocatalyst for enhanced solar fuels generation.
结构-活性关系对增强光催化性能起着至关重要的作用,然而,精确控制过渡金属氧化物的相仍然是一个重大的挑战。在此,我们开发了二氧化钛催化剂修饰的二维层状Mn3O4,以研究锰氧化物相对光催化CO2还原活性的影响。我们通过改变二氧化钛前驱体的量来优化氧化锰相。在合成反应中,TiCl4是决定氧化锰氧化态的关键因素。我们发现Mn3O4是光催化CO2还原的最佳相,Mn3O4/TiO2的光催化CO2还原性能分别比原始TiO2和Mn3O4提高20.1倍和7.8倍。光催化活性的提高与氧化锰的相态、载流子分离的增强和载流子寿命的延长有关。原位x射线吸收近边结构(XANES)证实了光催化CO2还原条件下氧化态的变化。此外,通过漫反射红外傅立叶变换光谱(DRIFTS)原位分析,提出了光催化机理。本研究为过渡金属氧化物基光催化剂的氧化态调控提供了一种有效的设计策略。
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引用次数: 0
Mechanisms of CO2 flooding front migration and injection-production regulation in heterogeneous reservoirs: A large-scale visual physical simulation study 非均质油藏CO2驱前运移及注采调控机理:大规模可视化物理模拟研究
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-01-21 DOI: 10.1016/j.jcou.2026.103339
Yutong Yan , Weifeng Lyu , Hongwei Yu , Wenfeng Lv , Shumin Ni
The unclear migration mechanisms of CO2 flooding fronts in heterogeneous reservoirs significantly constrain the efficiency enhancement of CCUS-EOR technology. This study, employing a self-designed large-scale two-dimensional visual physical model, systematically reveals for the first time the dominant control mechanism of interlayer spatial configuration on channeling pathways and the laws of injection-production regulation. Experiments demonstrate that when gas is injected on the side with a developed interlayer, CO2 preferentially migrates horizontally along the high-permeability layer and, after breakthrough, channels laterally into the low-permeability layer through the non-interlayer interface. Conversely, gas injection on the non-interlayer side induces vertical channeling. The mode of “gas injection at the non-interlayer end + oil production at the interlayer end” coupled with early soaking expanded the miscible zone by 29.81 % and achieved a total recovery factor of 91.04 %. Although increasing the pressure difference in the low-permeability layer by 1.5 times can forcibly initiate oil mobilization, channeling must be suppressed to avoid inter-layer imbalance. The evolution of the miscible zone exhibits a two-stage characteristic of “synergistic growth - competitive substitution”: dominated by mass transfer-displacement synergy before breakthrough, and by gas channeling and phase competition afterwards. The high-permeability layer readily forms an arc-shaped miscible enrichment zone, while the low-permeability layer exhibits narrow, strip-like expansion limited by mass transfer. Future work needs to focus on enhancing dynamic identification of the miscible zone, optimizing soaking timing, and combining numerical simulation to study the influence of interlayer spatial configuration on inter-layer channeling. These results provide key experimental evidence for CCUS-EOR development in heterogeneous reservoirs, promoting the advancement of inter-layer conflict regulation from mechanistic understanding to engineering optimization.
非均质油藏中CO2驱前沿运移机制不明确,严重制约了CCUS-EOR技术的效率提升。本研究采用自行设计的大尺度二维可视化物理模型,首次系统揭示了层间空间构型对窜流路径的主导控制机制和注采调节规律。实验表明,在夹层发育的一侧注气时,CO2优先沿高渗透层水平运移,突破后通过非夹层界面向低渗透层横向运移。相反,非层间侧的注气会引起垂直通道。采用“非层间端注气+层间端 采油”的模式,再加上早期浸泡,可将混相层扩大29.81 %,总采收率达到91.04 %。虽然将低渗透层压差提高1.5倍可以强制启动石油动员,但必须抑制窜流,以避免层间不平衡。混相带的演化呈现出“协同生长-竞争替代”的两个阶段特征:突破前以传质-驱替协同为主,突破后以气窜和相竞争为主。高渗层易形成弧形混相富集带,低渗层受传质限制呈窄条状扩张。今后的工作需要加强对混相带的动态识别,优化浸泡时间,并结合数值模拟研究层间空间构型对层间通道的影响。这些结果为非均质储层CCUS-EOR开发提供了关键的实验依据,促进了层间冲突调控从机理认识向工程优化的推进。
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引用次数: 0
Parametric study of CO2 capture and thermal energy storage in a CaO/CaCO3 bubbling fluidized bed with polydisperse particles 多分散颗粒CaO/CaCO3鼓泡流化床CO2捕集与储热参数研究
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-02-06 DOI: 10.1016/j.jcou.2026.103342
Liangsheng He , Shengnan Yan , Zhenggui Li , Fang Chen , Qin Zhao , Hongteng Wu , Yawei Bai , Xiaolin Yang
The CaO/CaCO3 cycle system holds broad application prospects in high-temperature processes such as thermal chemical energy storage for concentrated solar power generation and CO2 capture and utilization. However, most numerical studies typically employ calcium-based particles of a single particle size, making it difficult to reflect the influence of particle size distribution on fluidization and reaction behaviour within actual systems. To elucidate the fluidization and reaction characteristics of CaO/CaCO3 in bubbling fluidized beds, this study employs polydisperse calcium-based particles as the research subject. Numerical simulations incorporating chemical reactions are conducted to investigate particle fluidization behaviour under varying gas velocities, inlet CO2 volume fractions, and dynamic operating conditions from a parameterisation perspective. By comparing different particle size combinations, characteristic parameters such as bed solid content distribution, time-averaged CO2 concentration, time-averaged axial solid content, and time-averaged velocity were analysed. Results indicate that at constant gas velocity, the bed’s CO2 adsorption efficiency gradually decreases as particle size increases from 75 μm to 136 μm. In the mixed-particle-size system, at the same gas velocity, the CaCO3 solid content in the single-particle-size bed was slightly lower than that in the mixed-particle-size bed, while the CaO solid content was higher than that in the mixed-particle-size bed. Under different inlet CO2 concentration conditions, higher CO2 concentrations led to decreases in the bed's time-averaged velocity and time-averaged axial solid content. Considering particle temperature distribution, CO2 adsorption efficiency, CaO conversion rate, and energy storage density comprehensively, the calcium-based particle system demonstrated superior overall performance when the inlet CO2 volume fraction was 0.85.
CaO/CaCO3循环系统在聚光太阳能发电热化学储能、CO2捕集利用等高温工艺中具有广阔的应用前景。然而,大多数数值研究通常采用单一粒径的钙基颗粒,难以反映粒径分布对实际系统内流化和反应行为的影响。为了阐明CaO/CaCO3在鼓泡流化床中的流态化及反应特性,本研究以多分散钙基颗粒为研究对象。结合化学反应的数值模拟从参数化的角度研究了不同气体速度、进口二氧化碳体积分数和动态操作条件下颗粒流化行为。通过对比不同粒径组合,分析了床层固含量分布、时间平均CO2浓度、时间平均轴向固含量、时间平均流速等特征参数。结果表明:当气速恒定时,随着粒径从75 μm增大到136 μm,床层对CO2的吸附效率逐渐降低;在混合粒度系统中,在相同气速下,单粒度床的CaCO3固含量略低于混合粒度床,而CaO固含量高于混合粒度床。在不同的进口CO2浓度条件下,较高的CO2浓度导致床层时间平均速度和时间平均轴向固含量降低。综合考虑颗粒温度分布、CO2吸附效率、CaO转化率和储能密度等因素,当进口CO2体积分数为0.85时,钙基颗粒体系整体性能更优。
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引用次数: 0
Boosting CO₂ utilization in dry methane reforming using a two-stage DC-pulsed spark cold plasma reactor 利用两级直流脉冲火花冷等离子体反应器提高干甲烷重整中CO₂的利用率
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-02-02 DOI: 10.1016/j.jcou.2026.103343
P. Majidi , S. Jafarmadar , S. Fathi
The dry methane reforming process holds the potential to convert the greenhouse gas carbon dioxide into high-value-added fuels and chemicals, presenting broad application prospects in the fields of environmental protection and renewable energy. In this study, a two-stage pulsed discharge cold plasma reactor was experimentally investigated at ambient temperature and atmospheric pressure. The primary products of this process were syngas (CO and H₂), with smaller quantities of C₂Hᵧ compounds (y = 2, 4, or 6) also produced as by-products. This research aims to examine and compare a single-stage plasma system with a two-stage system. The results demonstrate that a significant improvement in methane conversion and hydrogen selectivity is achieved when the plasma energy is discharged across two stages. This performance enhancement is attributed to the presence of hydrogen generated in the second plasma stage. These findings indicate that plasma power alone is not the sole factor determining optimal performance; rather, the method of its delivery can profoundly influence the conversion of methane and carbon dioxide, product yields, and energy conversion efficiency. In this configuration, the hydrogen produced in the first stage promotes the generation of radicals in the second stage, consequently increasing both conversion rates and energy efficiency despite the constant total plasma energy input. Another contributing factor to the performance improvement is that a larger, more homogeneous gas volume is exposed to the pulsed discharge in the second plasma stage, which can lead to an increased effective gas residence time within the plasma.
甲烷干式重整工艺具有将温室气体二氧化碳转化为高附加值燃料和化学品的潜力,在环保和可再生能源领域具有广阔的应用前景。在常温常压条件下,对两级脉冲放电冷等离子体反应器进行了实验研究。该过程的主要产物是合成气(CO和H₂),少量的C₂Hᵧ化合物(y = 2,4或6)也作为副产物产生。本研究旨在检验和比较单级等离子体系统和两级等离子体系统。结果表明,当等离子体能量跨两个阶段放电时,甲烷转化率和氢气选择性显著提高。这种性能的增强是由于在第二等离子体阶段产生的氢的存在。这些发现表明,等离子体功率本身并不是决定最佳性能的唯一因素;相反,它的输送方法可以深刻地影响甲烷和二氧化碳的转化、产品产量和能量转换效率。在这种结构中,第一阶段产生的氢促进了第二阶段自由基的产生,从而提高了转化率和能量效率,尽管总等离子体能量输入不变。另一个有助于提高性能的因素是,在第二等离子体阶段,更大、更均匀的气体体积暴露在脉冲放电中,这可以导致等离子体内有效气体停留时间的增加。
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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 Pub Date : 2026-03-01 Epub 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
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 Pub Date : 2026-03-01 Epub 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 (Niδ⁻), 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@Na1.9K3.3Br(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
Trends and limits of CO2 capture in solid and liquid sorbents at standard conditions 标准条件下固体和液体吸附剂中CO2捕获的趋势和限制
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-02-09 DOI: 10.1016/j.jcou.2026.103338
Rohan Sartape , Rohit Chauhan , Samdavid Swaminathan , Ishita Goyal , Amey Thorat , Jindal K. Shah , Meenesh R. Singh
Carbon capture and storage (CCS) plays a critical role in achieving climate change mitigation targets, offering a pathway to decarbonize power generation, industrial processes, and heat production while addressing atmospheric CO2 removal. While CCS technologies are technically advanced, the widespread adoption of 100 % CO2 capture capacities such as 1 mol of CO2/mol of material and 1 g CO2/g storage (targeted by the DARPA, Defense Sciences Office, USA Govt.) has raised questions about the feasibility of achieving higher capture capacities. In the context of limiting global warming to 1.5°C, reaching 100 % CO2 capture capacity is increasingly necessary, with residual emissions requiring complementary carbon dioxide removal (CDR) technologies. This review exclusively focuses on the CO2 capture capacities of various sorbents under standard conditions, using different evaluation metrics. This study explores the performance of solid and liquid sorbents under standard conditions, analyzing factors including surface area, pore structure, solvent type, and functionalization to identify materials optimized for industrial-scale CCS applications. Emerging sorbents, including ILs, MOFs, COFs, POPs, DES, RCC, hybrid materials, and reactive sorbents, offer significant potential for enhanced selectivity and energy-efficient regeneration. Through a systematic assessment of gravimetric, volumetric, and molar capacities, the study provides insights into material efficiencies and trade-offs, offering guidance on optimizing sorbent selection for specific applications. The research advances understanding of scalable CCS technologies, contributing to global efforts to achieve net-zero emissions and address the pressing challenge of climate change.
碳捕集与封存(CCS)在实现减缓气候变化目标方面发挥着关键作用,为发电、工业过程和产热脱碳提供了一条途径,同时解决了大气中二氧化碳的去除问题。虽然CCS技术在技术上是先进的,但广泛采用100% %的二氧化碳捕获能力,如1 mol CO2/mol材料和1 g CO2/g存储(美国国防部高级研究计划局,国防科学办公室,美国政府的目标),已经提出了关于实现更高捕获能力可行性的问题。在将全球变暖限制在1.5°C的背景下,越来越有必要达到100% %的二氧化碳捕获能力,剩余排放需要补充二氧化碳去除(CDR)技术。本文主要介绍了不同吸附剂在标准条件下的CO2捕集能力,采用不同的评价指标。本研究探讨了固体和液体吸附剂在标准条件下的性能,分析了表面积、孔隙结构、溶剂类型和功能化等因素,以确定适合工业规模CCS应用的优化材料。新兴的吸附剂,包括ILs、mof、COFs、POPs、DES、RCC、杂化材料和反应性吸附剂,在提高选择性和节能再生方面具有巨大的潜力。通过对重量、体积和摩尔容量的系统评估,该研究提供了对材料效率和权衡的见解,为优化特定应用的吸附剂选择提供了指导。这项研究促进了对可扩展的CCS技术的理解,为全球实现净零排放和应对气候变化的紧迫挑战做出了贡献。
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引用次数: 0
CO2 and CH4 conversion in a rotating DC glow to arc plasma with big discharge gap 旋转直流辉光到大放电间隙电弧等离子体中CO2和CH4的转化
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-01 Epub Date: 2026-02-03 DOI: 10.1016/j.jcou.2026.103347
Samuel Jaro Kaufmann, Joe Quade, Johanna Buschmann, Haripriya Chinnaraj, Kai Peter Birke, Paul Rößner
In this work, we investigated large-volume, non-thermal discharges in CO₂/CH₄ mixtures with the aim of enabling energy-efficient plasma-based conversion. Building on the fundamental U–I characteristics of gas discharges, we showed how discharge extension and thermal management strongly affect the transition between glow and arc regimes. Using our Big Discharge-gap Glow-to-Arc (BDGTA) reactor, stable rotating discharges were realized at electrode gaps up to 40 mm. Depending on scale, plasma operation was achieved with average currents of 0.24–0.4 A and discharge voltages ranging from 1.5 kV (15 mm) to 4 kV (40 mm), corresponding to power levels between 400 and 1700 W. Optical diagnostics via high-speed camera confirmed the glow-like nature and the dynamics of the elongated discharges. Performance analysis revealed maximum energy efficiencies of 68 % (60 % CO2, 40 % CH4) and 60 % for 50/50 mixtures, with conversions up to 68 %. Carbon deposition in methane-rich mixtures was identified as a key challenge but can be mitigated through process adjustments like CO₂ recycling. Replacing ballast resistors with power-electronics plasma control minimized energy losses and ensured regime stability. Overall, the BDGTA reactor demonstrates that efficient, large-volume CO₂/CH₄ plasma conversion is feasible at atmospheric pressure, offering a pathway for sustainable electrification of chemical processes.
在这项工作中,我们研究了CO₂/CH₄混合物中的大体积非热放电,目的是实现节能的等离子体转化。基于气体放电的基本U-I特性,我们展示了放电扩展和热管理如何强烈影响辉光和电弧状态之间的过渡。利用我们的大放电间隙辉光转弧(BDGTA)反应器,在高达40 mm的电极间隙处实现了稳定的旋转放电。根据规模的不同,等离子体操作的平均电流为0.24-0.4 A,放电电压范围为1.5 kV(15 mm)至4 kV(40 mm),对应的功率水平在400至1700 W之间。通过高速相机进行的光学诊断证实了发光的性质和延长放电的动力学。性能分析显示,50/50混合物的最大能源效率为68% %(60 % CO2, 40 % CH4)和60 %,转化率高达68 %。富甲烷混合物中的碳沉积被认为是一个关键挑战,但可以通过CO₂回收等工艺调整来缓解。用电力电子等离子体控制取代镇流器电阻,最大限度地减少了能量损失,并确保了状态稳定性。总体而言,BDGTA反应器表明,在常压下,高效、大容量的CO₂/CH₄等离子体转化是可行的,为化学过程的可持续电气化提供了一条途径。
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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 Pub Date : 2026-03-01 Epub 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。
{"title":"Coupling DRM and NO reduction: A catalyst design strategy to control coking in Ni-based catalysts","authors":"Beatrice Senoner ,&nbsp;Andrea Osti ,&nbsp;Davide Chinello ,&nbsp;Giovanni Agostini ,&nbsp;Antonella Glisenti","doi":"10.1016/j.jcou.2026.103313","DOIUrl":"10.1016/j.jcou.2026.103313","url":null,"abstract":"<div><div>In the scenario of climate change, dry reforming of methane (DRM) is a well-studied reaction where CO<sub>2</sub> and CH<sub>4</sub> are converted into syngas, a mixture composed of CO and H<sub>2</sub> 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/CO<sub>2</sub>. Three Ni-impregnated catalysts are designed for this dual process: the chosen supports are γ-Al<sub>2</sub>O<sub>3</sub>, for its high dispersion and strong interaction with Ni, LaFeO<sub>3</sub>, for its NOx abatement properties and a mixed support LaFeO<sub>3</sub>-Al<sub>2</sub>O<sub>3</sub>. Only by combining the support properties in Ni/LaFeO<sub>3</sub>-Al<sub>2</sub>O<sub>3</sub> 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.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"105 ","pages":"Article 103313"},"PeriodicalIF":8.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145976257","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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 Pub Date : 2026-03-01 Epub 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。
{"title":"Molybdenum and tungsten carbides as catalysts for the reverse water gas shift reaction","authors":"Dahi Akmach ,&nbsp;Shang Jiang ,&nbsp;Anik Ashirwadam ,&nbsp;Malak El Kaddouri ,&nbsp;Samir H. Mushrif ,&nbsp;Serge Kaliaguine ,&nbsp;David S.A. Simakov","doi":"10.1016/j.jcou.2026.103327","DOIUrl":"10.1016/j.jcou.2026.103327","url":null,"abstract":"<div><div>For the sustainable utilization of carbon dioxide (CO<sub>2</sub>), 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 Mo<sub>2</sub>C 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 Mo<sub>2</sub>C promoted the formation of both CH<sub>4</sub> 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 CH<sub>4</sub>. 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.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"105 ","pages":"Article 103327"},"PeriodicalIF":8.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145976259","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Journal of CO2 Utilization
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