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Melamine-doped plastic-derived adsorbents for carbon capture: the influence of plastic type on textural properties and CO2 uptake. 用于碳捕获的三聚氰胺掺杂塑料衍生吸附剂:塑料类型对结构性能和二氧化碳吸收的影响。
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-03 DOI: 10.1016/j.jcou.2025.103262
Emmanuel Dan , Jake Sheriff , Alan J. McCue , Davide Dionisi , Claudia Fernández Martín
Melamine-doped adsorbents were synthesized from single PET and mixed plastics (MP) via the 2-pot method involving co-carbonisation with melamine, followed by KOH impregnation, and thermal activation. Under dynamic conditions at 25 °C and 1 bar, the PET- and MP-doped adsorbents exhibited CO₂ adsorption capacities of 1.98 and 1.59 mmol g−1, respectively, representing 10.6 and 17.8 % increase over their N-free counterparts (PET: 1.79 mmol g−1; MP: 1.35 mmol g−1). This also indicates that melamine doping had a greater impact on the adsorptive properties of the material derived from mixed plastics. Both doped adsorbents also showed excellent cyclic stability, maintaining regeneration efficiencies above 85 % over ten cycles, although slightly lower than the > 90 % seen in N-free adsorbents tested under the same regeneration conditions (100 °C with 50 mL min−1 of N2). Elemental analysis revealed higher nitrogen incorporation in N-MP (1.37 wt%) than in N-PET (0.24 wt%), despite an identical added amount of melamine, suggesting more efficient N-doping in the mixed plastics compared with PET. Although doped adsorbents exhibited lower surface area, total pore volume, and micropore volume compared to their N-free versions, they showed higher ultra-micropore volumes, which can enhance affinity for CO₂ adsorption at the pressure tested. Lastly, the type of plastic precursor had minimal effect on the adsorption mechanism or kinetics, as all adsorbents followed the Sips isotherm and Avrami’s kinetic models.
以单个PET和混合塑料(MP)为原料,采用三聚氰胺共碳化、KOH浸渍、热活化的两锅法制备了三聚氰胺掺杂吸附剂。在25°C和1 bar的动态条件下,掺杂PET和MP的吸附剂的CO₂吸附量分别为1.98和1.59 mmol g−1,比不掺杂n的吸附剂(PET: 1.79 mmol g−1;MP: 1.35 mmol g−1)提高了10.6和17.8 %。这也表明三聚氰胺掺杂对混合塑料衍生材料的吸附性能有较大的影响。两种掺杂吸附剂也表现出优异的循环稳定性,在10个循环中保持85 %以上的再生效率,尽管略低于在相同再生条件下(100°C, 50 mL min−1 N2)测试的无n吸附剂的>; 90 %。元素分析显示,尽管三聚氰胺的添加量相同,N-MP中的氮掺入率(1.37 wt%)高于N-PET(0.24 wt%),这表明与PET相比,混合塑料中的n掺杂效率更高。虽然与不含氮的吸附剂相比,掺杂的吸附剂的比表面积、总孔隙体积和微孔体积更小,但它们的超微孔体积更高,这可以增强压力测试下对CO₂的吸附能力。最后,塑料前驱体的类型对吸附机理或动力学的影响很小,因为所有吸附剂都遵循Sips等温线和Avrami的动力学模型。
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引用次数: 0
Reactive dyeing of flax fabric using supercritical carbon dioxide with organic bases 超临界二氧化碳与有机碱对亚麻织物的活性染色
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-03 DOI: 10.1016/j.jcou.2025.103259
Tieming Fan, Shang Shang
The dyeing feasibility of flax fabric was investigated with organic bases utilizing a pyrimidine-base reactive dye in supercritical carbon dioxide (Sc-CO2). Effects of organic base, pickup rate, temperature, pressure, time, and concentration of organic base on the color strength (K/S) and fixation rates of the flax fabric were investigated. The results illustrated that successful dyeing was achieved due to the nucleophilic substitution reaction of difluoro monochloro pyrimidine group in Reactive Dark Blue KM-GR and hydroxyl functional groups in flax. K/S values of the dyed flax samples were enhanced when the dyeing parameters changed. An optimized dyeing procedure of flax fabrics was suggested with a pickup of 100 %, a temperature of 90 ℃, a pressure of 18 MPa, a time of 90 min, and an organic base concentration of 10 g/L in Sc-CO2. Additionally, the colorfastness of the dyed samples, including rubbing, washing, and light valued over 5 was presented. In general, this work combines the synergistic advantages of fabric pre-treatment and Sc-CO2 dyeing to explore a green dyeing process with low water consumption and high dye uptake.
以一种嘧啶基活性染料为原料,研究了有机碱在超临界二氧化碳(Sc-CO2)中对亚麻织物染色的可行性。考察了有机碱、起绒率、温度、压力、时间和有机碱浓度对亚麻织物色强(K/S)和固绒率的影响。结果表明,活性深蓝KM-GR中的二氟一氯嘧啶基团与亚麻中的羟基官能团发生亲核取代反应,可成功染色。染色后亚麻样品的K/S值随染色参数的变化而增大。提出了亚麻织物染色的最佳工艺条件:上染率为100% %,温度为90 ℃,压力为18 MPa,时间为90 min, Sc-CO2中有机碱浓度为10 g/L。此外,还介绍了染色样品的色牢度,包括摩擦,洗涤和光照值超过5。总的来说,本工作结合了织物前处理和Sc-CO2染色的协同优势,探索了一种低用水量、高染料吸收率的绿色染色工艺。
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引用次数: 0
Feasibility study for developing bacteria-based carbon-neutral mortar-Evaluation of bacterial CO2 capture performance 开发细菌基碳中性砂浆的可行性研究——细菌CO2捕获性能评价
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-03 DOI: 10.1016/j.jcou.2025.103264
Min-Hee Won , Ji-Won Hwang , Keun-Hyeok Yang , Sang-Seob Lee
This study explores the feasibility of a novel bacteria-based mortar and concrete capable of capturing atmospheric CO2 throughout their service life without additional facilities. Isolated bacterial strains–Rhodopseudomonas palustris, Sphingobacterium multivorum, and Lysinibacillus sphaericus–were immobilized on porous expanded vermiculite to preserve viability under the extreme conditions of hardened concrete. The immobilized bacteria exhibited robust CO2 uptake under diverse exposure conditions, including light/dark cycles, relative humidity from 60 % to 99 %, and temperatures ranging from 5 °C to 35 °C. Even at 5 °C, CO2 capture performance was maintained at more than 42 % of that achieved at 20–35 °C. The bacteria-immobilizing expanded vermiculites outperformed biochar specimens, exhibiting significantly higher CO2 capture capacities and a much faster rate of CO2 sequestration, even at the exposure temperature of 5 °C. Viable cell counts confirmed bacterial populations increased by 2.3–3.3 times after CO2 exposure, indicating continued growth and activity. These findings establish a scientific basis for integrating living bacterial systems into construction materials as a pathway toward carbon-neutrality. Future research will focus on developing biological mortars, evaluating their mechanical and durability properties, and ensuring environmental safety. The proposed approach offers a promising direction for transforming concrete into a sustainable material capable of active CO2 capture, potentially revolutionizing the construction industry’s role in climate change mitigation.
本研究探索了一种新型细菌基砂浆和混凝土的可行性,该砂浆和混凝土能够在其整个使用寿命内捕获大气中的二氧化碳,而无需额外的设施。孤立的细菌strains-Rhodopseudomonas palustris, Sphingobacterium multivorum, Lysinibacillus sphaericus-were固定在多孔膨胀蛭石保护生存的极端条件下硬化混凝土。在不同的暴露条件下,包括光照/黑暗循环,相对湿度为60% %至99 %,温度为5°C至35°C,固定化细菌表现出强劲的二氧化碳吸收。即使在5°C时,CO2捕获性能也保持在20-35°C时的42% %以上。细菌固定化膨胀蛭石的性能优于生物炭样品,即使在5°C的暴露温度下,也表现出更高的CO2捕获能力和更快的CO2固存速度。活细胞计数证实,CO2暴露后细菌数量增加了2.3-3.3倍,表明持续生长和活动。这些发现为将活细菌系统整合到建筑材料中作为实现碳中和的途径奠定了科学基础。未来的研究将集中在开发生物砂浆、评估其力学和耐久性以及确保环境安全等方面。提出的方法为将混凝土转化为能够主动捕获二氧化碳的可持续材料提供了一个有希望的方向,可能会彻底改变建筑行业在减缓气候变化方面的作用。
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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 Pub 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 gcat min gHDPE−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 gcat min gHDPE−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 gH2 gHDPE−1 has been obtained at 650 °C with a space time of 25 gcat min gHDPE−1 and CO2/C molar ratio of 1.5, attaining a syngas production of 4.7 gsyngas gHDPE−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
Analysis of CO2 emissions from natural gas-fired power plants and an emission control strategy 天然气发电厂二氧化碳排放分析及排放控制策略
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-31 DOI: 10.1016/j.jcou.2025.103256
Mustafizur Rahman , Faijunnesa Rashid
The quantification, prediction, and reduction strategies of CO2 emissions are essential for their negative impacts on health, the environment, and the global climate. This study analyzed CO2 emissions from Engine-based Natural gas-fired power plants and forecasted CO2 emissions. To quantify, analyze, and predict CO2 emissions using Error, Trend, and Seasonal (ETS), Trigonometric seasonality, Box-Cox transformation, ARMA errors, Trend and Seasonal components (TBATS), Auto-Regressive Integrated Moving Average (ARIMA), Holt, Holt-Winters and Extreme Learning Machine (ELM) modeling approaches have been adapted and selected the best model among them based on CO2 emissions data from natural gas-fired power plants. This paper introduced a new idea to reduce emissions by using exhaust to generate electricity. This study investigated the contribution of Exhaust Gas Boilers (EGB) to CO2 emission reductions and found in engine based Natural Gas fired power plants, it reduces on average 0.8–10 % of CO2 emissions using Waste Heat Recovery (WHR), and this reduction is dependent on engine load, but waste air or exhaust is still released into the atmosphere. This paper introduces a conceptual framework for Waste Air Recovery (WAR), a forward-looking approach that proposes utilizing post-EGB exhaust air in turbine systems for further efficiency gains and emissions reduction. While not evaluated empirically in this study, WAR is presented as a potential direction for future research.
二氧化碳排放的量化、预测和减少战略对其对健康、环境和全球气候的负面影响至关重要。本研究分析了以发动机为基础的天然气发电厂的二氧化碳排放量,并预测了二氧化碳排放量。利用误差、趋势和季节(ETS)、三角季节性、Box-Cox变换、ARMA误差、趋势和季节分量(TBATS)、自回归综合移动平均(ARIMA)、Holt、Holt- winters和极限学习机器(ELM)建模方法对二氧化碳排放进行量化、分析和预测,并根据天然气发电厂的二氧化碳排放数据从中选择最佳模型。本文介绍了一种利用废气发电来减少排放的新思路。本研究调查了废气锅炉(EGB)对二氧化碳减排的贡献,发现在以发动机为基础的天然气发电厂,使用废热回收(WHR)平均减少0.8-10 %的二氧化碳排放,这种减少取决于发动机负载,但废气或废气仍然释放到大气中。本文介绍了废气回收(WAR)的概念框架,这是一种前瞻性的方法,建议在涡轮系统中利用egb后废气来进一步提高效率和减少排放。虽然在本研究中没有进行实证评估,但WAR被认为是未来研究的一个潜在方向。
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引用次数: 0
Impact of fluctuating temperature and pressure of injected CO2 on adsorption performance in a packed-bed reactor: A CFD-based study 注入二氧化碳的温度和压力波动对填充床反应器吸附性能的影响:基于cfd的研究
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-29 DOI: 10.1016/j.jcou.2025.103253
Ali M. Sefidan, Jari Vepsäläinen
This study investigates the influence of oscillatory inlet conditions on CO2 adsorption performance and energy efficiency in a packed-bed reactor using Computational Fluid Dynamics (CFD) modelling. Baseline operating values of 3 bar and 20 °C were selected as representative conditions, and systematic oscillations in pressure (AP=±0.2 to 2 bar) and temperature (AT=±2 to 10 °C) were imposed at frequencies of 0.001 to 0.01 Hz. Three forcing patterns – snusoidal, triangular, and step changes – were considered and compared to steady operation. The results show that pressure oscillations dominate the dynamic adsorption response: large amplitudes (±2 bar) reduce average CO2 uptake by up to 16% and increase specific energy consumption by 18% relative to steady-state. Temperature oscillations alone have negligible impact under the present baseline, as symmetric forcing cancels over each cycle; however, when temperature oscillations are coupled with pressure swings, they significantly affect the cooling energy load. Among waveform types, triangular oscillations achieve the most favourable balance of adsorption performance and energy demand, while step changes lead to the poorest efficiency. Overall, the findings demonstrate that oscillatory injection conditions generally reduce adsorption performance, with pressure fluctuations exerting the strongest influence, underscoring the importance of pressure-stabilizing strategies for efficient CO2 capture.
利用计算流体动力学(CFD)模型研究了振荡进口条件对填料床反应器CO2吸附性能和能效的影响。选择3 bar和20°C的基线工作值作为代表性条件,并在0.001至0.01 Hz的频率下施加压力(AP=±0.2至2 bar)和温度(AT=±2至10°C)的系统振荡。考虑了三种强迫模式——正弦、三角形和阶跃变化,并与稳定运行进行了比较。结果表明,压力振荡主导了动态吸附响应:相对于稳态,大振幅(±2 bar)可使平均二氧化碳吸收量减少16%,比能量消耗增加18%。在目前的基线下,温度振荡本身的影响可以忽略不计,因为对称强迫在每个周期内都会取消;然而,当温度波动与压力波动耦合时,它们会显著影响冷却能量负荷。在波形类型中,三角振荡达到了吸附性能和能量需求的最佳平衡,而阶跃变化导致效率最差。总体而言,研究结果表明,振荡注入条件通常会降低吸附性能,其中压力波动的影响最大,强调了压力稳定策略对有效捕获CO2的重要性。
{"title":"Impact of fluctuating temperature and pressure of injected CO2 on adsorption performance in a packed-bed reactor: A CFD-based study","authors":"Ali M. Sefidan,&nbsp;Jari Vepsäläinen","doi":"10.1016/j.jcou.2025.103253","DOIUrl":"10.1016/j.jcou.2025.103253","url":null,"abstract":"<div><div>This study investigates the influence of oscillatory inlet conditions on CO<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> adsorption performance and energy efficiency in a packed-bed reactor using Computational Fluid Dynamics (CFD) modelling. Baseline operating values of 3 bar and 20 °C were selected as representative conditions, and systematic oscillations in pressure (<span><math><mrow><msub><mrow><mi>A</mi></mrow><mrow><mi>P</mi></mrow></msub><mo>=</mo><mo>±</mo><mspace></mspace><mn>0</mn><mo>.</mo><mn>2</mn></mrow></math></span> to 2 bar) and temperature (<span><math><mrow><msub><mrow><mi>A</mi></mrow><mrow><mi>T</mi></mrow></msub><mo>=</mo><mo>±</mo><mspace></mspace><mn>2</mn></mrow></math></span> to 10 °C) were imposed at frequencies of 0.001 to 0.01 Hz. Three forcing patterns – snusoidal, triangular, and step changes – were considered and compared to steady operation. The results show that pressure oscillations dominate the dynamic adsorption response: large amplitudes (<span><math><mo>±</mo></math></span>2 bar) reduce average CO<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> uptake by up to 16% and increase specific energy consumption by 18% relative to steady-state. Temperature oscillations alone have negligible impact under the present baseline, as symmetric forcing cancels over each cycle; however, when temperature oscillations are coupled with pressure swings, they significantly affect the cooling energy load. Among waveform types, triangular oscillations achieve the most favourable balance of adsorption performance and energy demand, while step changes lead to the poorest efficiency. Overall, the findings demonstrate that oscillatory injection conditions generally reduce adsorption performance, with pressure fluctuations exerting the strongest influence, underscoring the importance of pressure-stabilizing strategies for efficient CO<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> capture.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103253"},"PeriodicalIF":8.4,"publicationDate":"2025-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145412419","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
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 Pub 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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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 Pub 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
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 Pub 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 Ca2 + –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
Is solid calcium looping a scalable technology for mega-ton carbon dioxide removal? 固体钙环是一种可扩展的去除百万吨二氧化碳的技术吗?
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-28 DOI: 10.1016/j.jcou.2025.103255
M.M. Paulsen, S.G.R. Nielsen, F.J. Tilsted, T.H. Pedersen
Atmospheric CO2 removal at Gton scale is necessary to limit global temperature rise. This study provides essential insights into the energy, area, and water requirements of solid calcium looping for large-scale CO2 removal, combining experimental results with an upscaled system context. Thermogravimetric analysis (TGA) characterizes the products, while scanning electron microscopy (SEM) qualitatively assesses sorbent performance. Experiments in a climate chamber focus on carbonation kinetics, varying relative humidity, temperature, and slaking ratios.
Results demonstrate that relative humidity above 70 % significantly enhances carbonation rates, favoring the placement of facilities in high-humidity locations. The optimal slaking ratio is identified as one mole of water per mole of CaO. Carbonation at 20 °C yields faster reaction kinetics than at 12 °C, with both temperatures achieving a carbonation degree of 66 mol.% in three and four days, respectively. Lower temperatures require a larger area to achieve similar annual capture rates. Cyclic testing shows stable capture capacity and carbonation kinetics over nine cycles.
For a one-million-ton-per-year capture unit, the process requires 4.9–6.2 GJ/tonCO2 for electric heating, with air contactor areas reduced to 0.08–0.12 km2 using vertically stacked sorbent trays. Water consumption reaches 0.7 tonH2O/tonCO2 at the optimal slaking ratio but can be minimized in high-humidity, water-scarce locations by omitting slaking, at the expense of larger area requirements.
While only northern Europe currently meets the conditions for implementing the technology, considering both electricity grid CO2 intensity and weather, the potential of solid calcium looping for large-scale CO2 removal remains promising, warranting further exploration of logistics and practicalities in real-world applications.
在吨级尺度上去除大气中的二氧化碳是限制全球气温上升的必要条件。本研究结合实验结果和升级的系统背景,为大规模去除CO2的固体钙环的能量、面积和水需求提供了重要的见解。热重分析(TGA)表征产品,而扫描电子显微镜(SEM)定性评估吸附剂的性能。在气候室的实验集中在碳化动力学,改变相对湿度,温度,和脱水比。结果表明,70%以上的相对湿度显著提高了碳酸化率,有利于将设施放置在高湿度的位置。最佳熟化比确定为1mol水/ 1mol CaO。在20°C下碳化比在12°C下碳化产生更快的反应动力学,两种温度下分别在3天和4天内达到66 mol.%的碳化度。较低的温度需要更大的面积才能达到相似的年捕获率。循环测试表明,在9个循环中,捕获能力和碳化动力学稳定。对于100万吨/年的捕集装置,该过程需要4.9-6.2 GJ/吨二氧化碳用于电加热,使用垂直堆叠的吸附剂托盘将空气接触器面积减少到0.08-0.12 km2。在最佳熟化比下,用水量达到0.7吨水/吨二氧化碳,但在高湿度、缺水的地区,可以通过忽略熟化来最小化用水量,但代价是需要更大的面积。虽然目前只有北欧符合实施该技术的条件,但考虑到电网的二氧化碳强度和天气,固体钙环法大规模去除二氧化碳的潜力仍然很有希望,需要进一步探索现实应用中的物流和实用性。
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引用次数: 0
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Journal of CO2 Utilization
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