Carbon Capture Science & Technology最新文献_第2页

Development of a fluidized bed reactor for catalytic dry reforming of methane with CO2 甲烷- CO2催化干重整流化床反应器的研制

Carbon Capture Science & Technology

Pub Date : 2025-11-13 DOI: 10.1016/j.ccst.2025.100540

Shihang Yu , Cong Li , Li Lyu , Rongsheng Cai , Lifeng Xiao , Yilai Jiao , Huanhao Chen , Xiaoxia Ou , Xiaoyang Wei , Xaiolei Fan

Experimental studies of dry reforming of methane (DRM) under bubbling regime in the thermal fluidized bed reactors (FBRs) remain limited. In this study, a thermal FBR was developed, and catalytic DRM was systematically evaluated. Nickel-supported catalysts (Ni/FCC) were prepared via a wet impregnation method using commercial fluid catalytic cracking (FCC) particles, and their physicochemical properties were comprehensively characterized. Detailed fluidization behaviour was investigated using pressure drop fluctuations and discrete wavelet transformation (DWT), revealing a transition velocity (Uc) between bubbling and turbulent regimes in the FBR (under the conditions relevant to DRM), which was found to decrease with increasing temperature. DRM performance of Ni/FCC was assessed under various reaction temperatures (600–800 °C), gas velocities (0.1–0.2 m/s), and preheating conditions. Optimal operation in the bubbling regime (800 °C, 0.1 m/s) enabled CO₂ and CH₄ conversions of 57% and 41%, respectively, with an H₂/CO ratio of 0.67. Comparative studies demonstrated that the packed bed reactor (PBR) achieved higher conversions and better H₂/CO ratios (∼0.96), attributed to its plug flow characteristics, whereas the FBR exhibited lower conversions due to gas back mixing and reactant bypassing. Nevertheless, the Ni/FCC catalyst exhibited good thermal stability and negligible deactivation in both reactor configurations during 20 h of continuous operation. These findings provide practical insights into the design, operation, and catalytic behaviour of FBR systems for industrial DRM applications.

热流化床反应器（FBRs）鼓泡状态下甲烷干重整（DRM）的实验研究仍然有限。本研究开发了一种热快堆，并对催化DRM进行了系统评价。以工业流体催化裂化（FCC）颗粒为原料，采用湿浸渍法制备了镍负载催化剂（Ni/FCC），并对其理化性能进行了全面表征。利用压降波动和离散小波变换（DWT）研究了详细的流化行为，揭示了快堆中鼓泡和湍流状态之间的过渡速度（Uc）（在与DRM相关的条件下），发现其随着温度的升高而降低。在不同的反应温度（600 ~ 800℃）、气速（0.1 ~ 0.2 m/s）和预热条件下，对Ni/FCC的DRM性能进行了评价。在鼓泡状态下（800℃，0.1 m/s）的最佳操作使CO2和CH4的转化率分别达到57%和41%，H2/CO比为0.67。对比研究表明，填料床反应器（PBR）由于其塞流特性，具有更高的转化率和更好的H2/CO比（~ 0.96），而快堆反应器由于气体回混和反应物旁路而具有较低的转化率。然而，Ni/FCC催化剂表现出良好的热稳定性，在两种反应器配置下连续运行20 h时，可以忽略失活。这些发现为工业DRM应用中FBR系统的设计、操作和催化行为提供了实用的见解。

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引用次数: 0

Graphene-doped membranes for direct air capture (m-DAC) of CO2 用于二氧化碳直接空气捕获（m-DAC）的石墨烯掺杂膜

Carbon Capture Science & Technology

Pub Date : 2025-11-13 DOI: 10.1016/j.ccst.2025.100541

Omnya Al-Yafiee , Priyanka Kumari , Christophe Castel , Ze-Xian Low , Lei Wang , Yichang Pan , Konstantinos Papadopoulos , Dionysios Vroulias , Theophilos Ioannides , George E. Romanos , Eric Favre , Georgios Karanikolos , Ludovic F. Dumée

Rising atmospheric CO₂ levels drive the urgent need for efficient capture technologies. Conventional methods such as amine-based absorption and solid desiccants are energy-intensive and costly. Membrane gas separation offers a promising alternative due to its process simplicity and potential cost reduction, though its application in Direct Air Capture (DAC) remains underexplored. Unlike cyclic sorbent-based DAC systems, membrane-based separation enables continuous CO2 capture without chemical regeneration steps. This approach offers a scalable, modular pathway for low-maintenance DAC operation. This study presents highly CO₂-selective and permeable polymeric membranes able to strip CO₂ from synthetic ambient air. The performance of the membranes was enhanced by incorporating amine-functionalized graphene oxide (GO) into micron-thin block-copolymer membranes, supporting interfacial engineering to increase CO₂ affinity and enhance flux via interstitial diffusion. The membranes achieved CO₂/N₂ selectivities of 68±2 and permeabilities of 21.27±0.5 GPU under DAC conditions (0.04 % v/v CO₂ in N₂). The stability of the performance in humid conditions up to 45 RH% was also tested and the selectivities found to remain on par with dry air testing, supporting the development of m-DAC as a viable route to support atmospheric CO₂ capture. A multi-stage membrane process simulation was also conducted to evaluate the scalability of the process, demonstrating its feasibility and cost for large-scale CO₂ capture.

不断上升的大气二氧化碳水平推动了对高效捕集技术的迫切需求。传统的方法，如胺基吸收和固体干燥剂是能源密集型和昂贵的。膜气体分离因其过程简单和潜在的成本降低而提供了一个有前途的替代方案，尽管其在直接空气捕获（DAC）中的应用仍未得到充分探索。与基于循环吸附剂的DAC系统不同，基于膜的分离可以在没有化学再生步骤的情况下连续捕获二氧化碳。这种方法为低维护DAC操作提供了可扩展的模块化途径。这项研究提出了高二氧化碳选择性和渗透性的聚合物膜，能够从合成的环境空气中去除二氧化碳。将胺功能化的氧化石墨烯（GO）加入到微米厚的嵌段共聚物膜中，支持界面工程，通过间隙扩散增加CO2亲和力和通量，从而提高膜的性能。在DAC条件下（0.04% v/v CO2 in N₂），膜的CO2/ n2选择性为68±2，渗透率为21.27±0.5 GPU。还测试了在高达45 RH%的潮湿条件下性能的稳定性，发现选择性与干燥空气测试保持一致，支持m-DAC作为支持大气二氧化碳捕获的可行途径的发展。此外，还进行了多阶段膜工艺模拟，以评估该工艺的可扩展性，证明其大规模CO2捕集的可行性和成本。

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引用次数: 0

Enabling e-fuels in Middle East and North Africa: Life cycle and techno-economic insights into CO2 capture and utilization 在中东和北非启用电子燃料：二氧化碳捕获和利用的生命周期和技术经济见解

Carbon Capture Science & Technology

Pub Date : 2025-11-08 DOI: 10.1016/j.ccst.2025.100538

Loiy Al-Ghussain , Bilal Rinchi , Mohammad Alrbai , Sameer Al-Dahidi , Zifeng Lu

This study evaluates the levelized cost and greenhouse gas (GHG) emission intensity of CO₂ capture and e-fuel production pathways across the Middle East and North Africa (MENA) region. Industrial point-source CO₂ capture shows favorable techno-economic performance, particularly from natural gas and oil processing facilities, with a regional weighted average cost of approximately 51 USD/tCO_2cap, making it a viable source of low-cost CO₂ for e-fuel production. Among MENA countries, Qatar, Oman, and the United Arab Emirates exhibit the lowest capture costs (38–44 USD/tCO_2cap), attributable to high emission volumes and low energy prices. The corresponding GHG emission intensity (EI) of point-source capture averages around 180 kgCO_2eq/tCO_2cap. Regarding e-fuel production, Fischer–Tropsch (FT) fuels are identified as the most expensive and carbon-intensive option, with average production costs exceeding 0.07 USD/MJ and EIs surpassing 30 gCO_2eq/MJ in most MENA countries. In contrast, ammonia synthesis offers the lowest emission intensity, ranging from 7.1 to 21.8 gCO_2eq/MJ depending on the energy source. Although none of the e-fuel pathways are currently cost-competitive with fossil fuels, industrial point-source CO₂ capture in the MENA region presents a promising near-term opportunity. Realizing this potential will require targeted policy measures, including the implementation of carbon pricing, the expansion of renewable energy capacity, and strategic infrastructure investments.

本研究评估了整个中东和北非地区二氧化碳捕集和电子燃料生产途径的平准化成本和温室气体（GHG）排放强度。工业点源二氧化碳捕获显示出良好的技术经济性能，特别是天然气和石油处理设施，区域加权平均成本约为51美元/吨二氧化碳cap，使其成为电子燃料生产的低成本二氧化碳的可行来源。在中东和北非国家中，由于高排放量和低能源价格，卡塔尔、阿曼和阿拉伯联合酋长国的捕集成本最低（38-44美元/吨二氧化碳上限）。点源捕获对应的温室气体排放强度（EI）平均在180 kgCO2eq/tCO2cap左右。在电子燃料生产方面，费托燃料（FT）被认为是最昂贵和碳密集的选择，在大多数中东和北非国家，平均生产成本超过0.07美元/兆焦耳，EIs超过30克二氧化碳当量/兆焦耳。相比之下，氨合成的排放强度最低，根据能源的不同，排放强度在7.1 ~ 21.8 gCO2eq/MJ之间。尽管目前没有一种电子燃料途径与化石燃料相比具有成本竞争力，但中东和北非地区的工业点源二氧化碳捕获提供了一个有希望的短期机会。实现这一潜力需要有针对性的政策措施，包括实施碳定价、扩大可再生能源产能和战略性基础设施投资。

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引用次数: 0

Energy-coupled CO2 capture–conversion via membrane–adsorption integration: Quantitative benchmarks and pilot-scale design 通过膜吸附整合的能量耦合CO2捕获转换：定量基准和中试规模设计

Carbon Capture Science & Technology

Pub Date : 2025-11-01 DOI: 10.1016/j.ccst.2025.100537

Hailing Ma , Xin Zhang , Yao Tong , Yew Mun Hung , Xin Wang

This review advances a unified framework for engineering low-energy, high-efficiency CO₂ capture–conversion platforms by co-designing membranes, adsorbents, and multi-field catalytic modules. We benchmark key performance indicators across materials and flowsheets—specific energy (kWh·t⁻¹-CO₂), capacity–selectivity trade-offs, cyclic stability, and space–time yield—and quantify integration benefits under harmonized boundaries (functional units, explicit ±compression, common base year).At 90 % capture efficiency with 10–15 % CO₂ feed, 40–60 % relative humidity, and a pressure drop of 0.2–0.4 bar, the membrane–adsorption architecture reduces specific energy by 30–40 % compared with membrane-only or adsorption-only baselines. It maintains both high capacity and selectivity and is compatible with VPSA or TDS regeneration. Design rules are distilled for Graphene Oxide (GO)/Reduced Graphene Oxide (rGO)–Metal Organic Framework (MOF) sorbents and Mixed-Matrix Membranes (MMMs), together with operating-window guidance that addresses H₂O/O₂ tolerance and interface matching. Along the conversion pathway, photocatalytic, thermocatalytic, and electrocatalytic subsystems are organized into a multi-field scheme in which structural and electronic-state tuning directs product selectivity and energy efficiency. A scenario-based Techno-Economic Analysis (TEA)/Life Cycle Assessment (LCA) compares centralized industrial flue gas, distributed biogas upgrading, and Direct Air Capture (DAC), with sensitivities to electricity/H₂ prices and sorbent lifetime. The resulting KPI toolkit and process maps aim to accelerate pilot-to-scale translation of integrated CO₂-to-chemicals systems.

本文通过共同设计膜、吸附剂和多场催化模块，提出了一种统一的低能耗、高效二氧化碳捕获转化平台的工程框架。我们对材料和流程的关键性能指标（比能（kWh·t−1-CO2）、产能选择性权衡、循环稳定性和时空产量）进行基准测试，并在协调边界（功能单位、明确±压缩、共同基准年）下量化集成效益。在90%的捕获效率下，10 - 15%的二氧化碳进给量，40 - 60%的相对湿度，0.2-0.4 bar的压降，与仅膜或仅吸附的基准相比，膜吸附结构降低了30 - 40%的比能。它保持高容量和选择性，并与VPSA或TDS再生兼容。本文总结了氧化石墨烯(GO)/还原氧化石墨烯(rGO) -金属有机框架（MOF）吸附剂和混合基质膜（MMMs）的设计规则，以及解决H2O/O2耐受性和界面匹配的操作窗口指导。沿着转化途径，光催化、热催化和电催化子系统被组织成一个多场方案，其中结构和电子状态调谐指导产物选择性和能量效率。基于场景的技术经济分析(TEA)/生命周期评估（LCA）比较了集中式工业烟气、分布式沼气升级和直接空气捕集（DAC），并对电力/H2价格和吸附剂寿命敏感。由此产生的KPI工具包和流程图旨在加速将集成的二氧化碳到化学品系统从试点到规模化的转换。

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引用次数: 0

CO2 reduction reimagined: From light-driven to electrocatalytic pathways with computational insight towards enhanced product selectivity 二氧化碳的减少重新设想：从光驱动到电催化途径与提高产品选择性的计算洞察力

Carbon Capture Science & Technology

Pub Date : 2025-10-30 DOI: 10.1016/j.ccst.2025.100536

Naveed Akhtar , Habib Ullah , Amir Zada , Shohreh Azizi , Muhammad Ateeq , Javed Ali Khan , Muhammad Ishaq Ali Shah , Mohammad Naeem , Muhammad Shakeel Khan , Zakir Ullah , Hyun You Kim

Transforming carbon dioxide (CO₂) into valuable fuels and chemicals through photocatalysis and electrocatalysis presents a sustainable approach to reducing carbon emissions and tackling global energy challenges. However, the major hurdles lie in the low activity and selectivity of these processes. This review critically analyzes the fundamental mechanisms and reaction pathways for CO₂ reduction, with a focus on photocatalytic and electrocatalytic approaches. Key factors influencing product selectivities, including the band structure of photocatalysts, light-excitation properties, charge carrier separation, and surface interactions, are thoroughly examined. We also emphasize recent advancements such as bandgap engineering, doping, nanostructure tailoring, and the use of innovative catalysts to enhance selectivity and efficiency. Unlike previous reviews that focus on either photocatalysis or electrocatalysis in isolation, this review offers a unified perspective on both system, whether highlighting comparative trends, mechanistic insights, and future research directions. This integrated and comprehensive analysis fills a critical gap in the current literature and expected to guide the development of next-generation catalytic systems for efficient and selective CO₂ conversion.

通过光催化和电催化将二氧化碳转化为有价值的燃料和化学品，是减少碳排放和应对全球能源挑战的可持续途径。然而，主要的障碍在于这些过程的低活性和选择性。本文分析了二氧化碳还原的基本机制和反应途径，重点介绍了光催化和电催化方法。影响产物选择性的关键因素包括光催化剂的能带结构、光激发性质、载流子分离和表面相互作用。我们还强调了最近的进展，如带隙工程，掺杂，纳米结构定制，以及使用创新催化剂来提高选择性和效率。不像以往的综述只关注光催化或电催化，这篇综述对这两个系统提供了统一的观点，无论是强调比较趋势，机理见解，还是未来的研究方向。这一综合和全面的分析填补了当前文献中的一个关键空白，并有望指导下一代高效和选择性CO2转化催化系统的发展。

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引用次数: 0

Dual moving bed calcium looping process: Optimizing CO2 capture efficiency and energy utilization 双移动床钙环工艺：优化CO2捕集效率和能源利用

Carbon Capture Science & Technology

Pub Date : 2025-10-28 DOI: 10.1016/j.ccst.2025.100535

Pengjun Cui , Godknows Dziva , Tingting Song , Sandeep Dhital , Shengping Wang , Liang Zeng

This study proposed a dual moving bed reactor configuration for the calcium looping (CaL) process, aiming to improve CO₂ capture efficiency and reduce the energy consumption. A multistage thermodynamic equilibrium model was developed to simulate the gas-solid countercurrent reactive flow pattern. A comparative study was conducted between the proposed dual moving bed (DMB) CaL system and the conventional dual fluidized bed (DFB) configuration. At an R_Ca/_C = 4, the gas-solid countercurrent moving bed carbonator can achieve a CO₂ capture efficiency exceeding 95 %, an improvement of over 3 % compared to the fluidized bed system operating at 650 °C. Internal countercurrent heat exchange of the MB carbonator increases the solid outlet temperature by approximately 60 °C, consequently reducing the calciner’s fuel consumption by 5.04 %. The gas-solid countercurrent flow in the calciner improved internal heat integration and further decreased fuel demand by 13.71 %. Thus, the DMB CaL system attained a calciner-specific energy consumption of 3.61 GJ/t CO₂, representing a 19.78 % reduction from the DFB CaL system. When integrated into a coal-fired power plant, the specific energy consumption for CO₂ avoided (SPECCA) is 2.40 GJ/t CO₂, an 8.40 % decrease compared to the DFB CaL process. This improvement enhances the techno-economic performance of the CaL process and highlights its potential for industrial CO₂ capture.

本研究提出了一种用于钙环（CaL）工艺的双移动床反应器配置，旨在提高CO2捕集效率，降低能耗。建立了多级热力学平衡模型来模拟气固逆流反应流态。对所提出的双移动床（DMB） CaL系统与传统的双流化床（DFB）配置进行了对比研究。在RCa/C = 4时，气固逆流移动床碳化器的CO2捕集效率超过95%，与运行在650℃的流化床系统相比，提高了3%以上。MB碳化器的内部逆流换热使固体出口温度提高了约60℃，从而使煅烧炉的燃料消耗降低了5.04%。煅烧炉内的气固逆流改善了内部热集成，进一步降低了13.71%的燃料需求。因此，DMB CaL系统的分解炉能耗为3.61 GJ/t CO2，比DFB CaL系统降低了19.78%。当集成到燃煤电厂时，避免二氧化碳的比能耗（SPECCA）为2.40 GJ/t CO2，与DFB CaL工艺相比降低了8.40%。这一改进提高了CaL工艺的技术经济性能，并突出了其在工业二氧化碳捕获方面的潜力。

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引用次数: 0

Enhancing CO2 electroreduction over iron-nitrogen-doped carbon catalysts by axial bromine coordination 轴向溴配位强化铁氮掺杂碳催化剂的CO2电还原

Carbon Capture Science & Technology

Pub Date : 2025-10-24 DOI: 10.1016/j.ccst.2025.100534

Jia Song , Long Shi , Jing Wei , Min Deng , Zikang Qin , Lin Yang , Junfeng Zheng , Wenju Jiang , Lu Yao , Zhongde Dai

Axial coordination engineering is a promising method to regulate the active sites of single atom catalysts (SACs) in electrochemical reduction of CO₂ (ECR) and further realize the manipulating of the electrocatalytic activity, selectivity, and stability of catalysts. Here, a facile post-synthetic modification strategy of metal exchange and heteroatom dopant was proposed to develop a single iron atom catalyst coordinated with four planar N atoms and one axial Br atom (denoted as Fe_x_-NCBr_y) for ECR to CO. By altering the operating conditions including pyrolysis temperature as well as dopant amount of Fe and Br, the optimized Fe₂₀-NCBr_0.3 catalyst acquired more surface-active sites and lower impedance, exhibiting an enhanced CO selectivity of 93.78 % with a CO reduction current density of -21.16 mA cm^-² at -0.9 V (vs. RHE). This work provides new possibilities for tuning the SACs coordination environment with an axial heteroatom for improved ECR performance.

轴向配位工程是调控电化学还原CO2过程中单原子催化剂活性位点，进而实现对催化剂电催化活性、选择性和稳定性的调控的一种很有前景的方法。本文提出了一种简单的金属交换和杂原子掺杂的合成后改性策略，开发了一种单铁原子与四个平面N原子和一个轴向Br原子（Fex-NCBry）配位的ECR - CO催化剂。通过改变热解温度、Fe和Br的掺杂量等操作条件，优化后的Fe20-NCBr0.3催化剂获得了更多的表面活性位点和更低的阻抗。在-0.9 V（相对于RHE）下，CO还原电流密度为-21.16 mA cm-2时，CO选择性提高了93.78%。这项工作为通过轴向杂原子调整SACs配位环境以提高ECR性能提供了新的可能性。

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引用次数: 0

District heating with negative emissions – direct air carbon capture and storage combined with small modular reactors 负排放区域供热-直接空气碳捕获和储存与小型模块化反应堆相结合

Carbon Capture Science & Technology

Pub Date : 2025-10-20 DOI: 10.1016/j.ccst.2025.100533

Heidi Kirppu, Miika Rämä, Esa Pursiheimo, Kati Koponen, Tomi J. Lindroos

Achieving Paris Agreement targets for climate change mitigation requires an urgent shift away from fossil fuels. In addition, negative emissions by permanently removing carbon dioxide from the atmosphere are required. Both targets require substantial amounts of carbon neutral electricity and heat production. While electricity can be produced and transferred over long distances, the heat production needs to be local. This study investigates an energy system integrating both carbon neutral heat production and carbon dioxide removal from the atmosphere. The system is modelled using the Backbone energy system modelling framework. The carbon neutral heat production in the study is based on small modular nuclear reactors (SMRs), large-scale thermal energy storages (TES), heat pumps (HPs) and electric boilers (EBs), and the carbon removal is implemented by direct air capture (DAC) combined with permanent geological storage. The studied technologies are integrated into a specific large-scale district heating system located in Northern Europe. The impact of outdoor temperature for the efficiency of the DAC process is considered, and the system integration potential with the district heating system is evaluated. The results show that high 70–90 % utilisation rates for both SMR and DAC units can be reached but depending on the case year and corresponding profiles for demand, outdoor temperature, electricity and carbon prices, a large variation in utilisation rates is observed. The variable CO₂ capture costs were between 115–126 €/t CO₂ in the modelled scenarios, and with higher OPEX values at the range 152–163€/tCO₂, and the limit price for economic viability considering the investment was calculated to be in the range of 209–223 €/tCO_2, with lower, and 233–246 €/tCO₂ with higher adsorbent costs. When not accounting the biogenic CO₂ emissions, the carbon negativity can be reached in the system in all the scenarios where the CO₂ price is over 150€/t and the number of DAC modules is at least 400. When accounting the biogenic CO₂ emissions, the carbon negativity can be reached only in scenarios with DAC capacity at 900 modules and CO₂ price at 180–200€/t.

要实现《巴黎协定》减缓气候变化的目标，就必须紧急放弃使用化石燃料。此外，需要通过永久清除大气中的二氧化碳来实现负排放。这两个目标都需要大量的碳中和电力和热能生产。虽然电力可以远距离生产和传输，但热量的生产需要在当地进行。本研究探讨了一种集碳中性产热和大气二氧化碳去除于一体的能源系统。该系统采用Backbone能源系统建模框架进行建模。研究中的碳中性热生产基于小型模块化核反应堆（SMRs）、大型热能储存（TES）、热泵（HPs）和电锅炉（EBs），碳的去除是通过直接空气捕获（DAC）和永久地质储存来实现的。所研究的技术被整合到位于北欧的一个特定的大型区域供热系统中。考虑了室外温度对DAC过程效率的影响，并对系统与区域供热系统的集成潜力进行了评估。结果表明，SMR和DAC单元的利用率都可以达到70 - 90%，但根据案例年份和相应的需求、室外温度、电力和碳价格，可以观察到利用率的巨大变化。在模拟情景中，可变CO2捕集成本在115-126欧元/吨CO2之间，在152-163欧元/吨CO2范围内，OPEX值较高；考虑到投资，经济可行性的极限价格在209-223欧元/吨CO2范围内，吸附剂成本较低，233-246欧元/吨CO2较高。在不考虑生物源性二氧化碳排放的情况下，在二氧化碳价格超过150欧元/吨且DAC模块数量至少为400的所有情况下，系统都可以达到碳负性。当计算生物源二氧化碳排放时，只有在DAC容量为900个模块，二氧化碳价格为180-200欧元/吨的情况下才能达到碳负性。

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引用次数: 0

Electroreduction of CO2 to C1 and C2 products on dual active sites 在双活性位点上电还原CO2生成C1和C2产物

Carbon Capture Science & Technology

Pub Date : 2025-10-17 DOI: 10.1016/j.ccst.2025.100532

Naimat Ullah , Munzir H. Suliman , Sikandar Khan , Zubair Ahmed Laghari , Guillermo Diaz-Sainz , Abdulmajeed Hendi , Wan Zaireen Nisa Yahya , Muhammad Usman

Electrochemical CO₂ reduction (eCO₂RR) is a promising method for transforming CO₂ emissions into useful multicarbon products. This study involved the synthesis and evaluation of CuS/ZnS nanocomposites with varying compositions (CuS: ZnS = 1:1, 2:1, and 1:2) in both H-type and flow-cell electrolyzers. The catalyst with a 2:1 CuS/ZnS ratio (S2) exhibited excellent performance, with a Faradaic efficiency (FE) of 60 % for C₁ products and approximately 20 % for C₂ products (C₂H₄) at a current density of −280 mA·cm⁻² in the flow-cell configuration. The flow-cell arrangement significantly enhanced catalytic activity, suppressed hydrogen evolution, and increased selectivity for CH₄ and C₂H₄ at greater negative potentials. Augmented ethylene production was ascribed to Cu-rich active sites promoting efficient C–C coupling and increased CO₂ accessibility at gas diffusion electrodes (GDEs), corroborated by low charge-transfer resistance (∼1 Ω·cm²). This work emphasizes the pivotal importance of catalyst composition and reactor design, showcasing the 2:1 CuS/ZnS catalyst in a flow-cell format as a scalable and effective method for sustainable CO₂ conversion to multicarbon fuels. Density functional theory (DFT) calculations further validated the experimental results by revealing favorable adsorption energies and interactions between the CuS/ZnS catalyst and key intermediates in the CO₂ conversion process.

电化学CO₂还原（eCO₂RR）是将CO₂排放转化为有用的多碳产品的一种很有前途的方法。本研究包括在h型和流动电池电解槽中合成和评价不同成分（cu: ZnS = 1:1, 2:1和1:2）的cu /ZnS纳米复合材料。cu /ZnS比为2:1的催化剂（S2）表现出优异的性能，在- 280 mA·cm⁻²的电流密度下，C₁产物的法拉第效率（FE）为60%，C2产物（C₂H₄）的法拉第效率（FE）约为20%。流动池结构显著提高了催化活性，抑制了析氢，并在较大的负电位下提高了CH₄和C₂H₄的选择性。乙烯产量的增加归因于富cu活性位点促进了高效的C-C偶联和气体扩散电极（GDEs）上CO 2的可及性，低电荷转移电阻（~ 1 Ω·cm²）证实了这一点。这项工作强调了催化剂组成和反应器设计的关键重要性，展示了流动电池形式的2:1 cu /ZnS催化剂是一种可扩展且有效的方法，可将二氧化碳可持续转化为多碳燃料。密度泛函理论（DFT）进一步验证了实验结果，揭示了cu /ZnS催化剂与CO₂转化过程中关键中间体之间的良好吸附能和相互作用。

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引用次数: 0

Attrition characteristics of Ca-based dual functional material in a micro fluidized-bed reactor for integrated CO2 capture and conversion ca基双功能材料在集成CO2捕集转化微流化床反应器中的磨损特性

Carbon Capture Science & Technology

Pub Date : 2025-10-15 DOI: 10.1016/j.ccst.2025.100531

Lei Liu, Hao Wang, Hanzi Liu, Zhiqiang Sun

Integrated carbon capture and utilization coupled with reverse water-gas shift reaction is a promising technology for converting captured CO₂ into value-added CO or syngas using a Ca-based dual functional material (DFM). However, existing Ca-based DMFs are primarily powder-based formulations, which poses challenges for their direct application in a real fluidized-bed reactor, and the attrition characteristics of DFM particles remain largely unexplored. Herein, a micro-fluidized-bed thermogravimetric analyzer coupled with a mass spectrometer (MFB-TGA-MS) was employed to investigate the attrition properties of three types of well-prepared Ca-based DFM particles under fluidizing conditions. It was found that Al-modified Ca-based DFM retained ∼6 mmol g^-1 CO₂ after 100 cycles, but high forming pressure reduced this to ∼4 mmol g^-1 while low pressure caused 2.24 % h^-1 physical loss in the first 10 cycles. Physical loss peaked within 20 cycles, while chemical loss occurred mainly before cycle 40 for the DFM without Al and shifted to cycles 40–80 with Al. SEM and TEM confirmed that the Al skeleton is beneficial for reducing the chemical loss via suppressing the sintering of Ni and CaO. However, high pellet-forming pressure would lessen the pore structure, hindering the volume change during the capture and hydrogenation processes. Finally, the integrated carbon capture and utilization - reverse water gas shift (ICCU-RWGS) performance was analyzed over a wide range of CO₂ and H₂ partial pressures. Decoupling of DFM particle attrition into chemical loss and physical loss provides insight to develop a highly efficient DFM particle.

综合碳捕集与利用与逆水气转换反应相结合是一种很有前途的技术，利用ca基双功能材料（DFM）将捕获的二氧化碳转化为增值的CO或合成气。然而，现有的ca基DMFs主要是粉状配方，这对其在实际流化床反应器中的直接应用提出了挑战，并且DFM颗粒的磨损特性在很大程度上仍未被探索。本文采用微流化床热重分析仪-质谱联用仪（MFB-TGA-MS）研究了三种制备好的ca基DFM颗粒在流化条件下的摩擦性能。结果发现，经过100次循环后，al改性ca基DFM保留了~ 6 mmol g-1 CO2，但高成型压力将其降低到~ 4 mmol g-1，而低压在前10次循环中造成2.24%的h-1物理损失。物理损失在20个循环内达到峰值，而化学损失主要发生在不含Al的DFM的第40循环之前，并转移到含有Al的第40 - 80循环。SEM和TEM证实，Al骨架通过抑制Ni和CaO的烧结有利于减少化学损失。然而，高成球压力会降低孔隙结构，阻碍捕获和加氢过程中的体积变化。最后，在较宽的CO2和H2分压范围内分析了碳捕集利用-反水气转换（ICCU-RWGS）的综合性能。将DFM颗粒磨损解耦为化学损失和物理损失，为开发高效的DFM颗粒提供了见解。

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