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Enhanced performance of oxygen vacancies on CO adsorption and activation over different phases of ZrO

《能源前沿（英文）》 2023年第17卷第4期页码 545-554 doi: 10.1007/s11708-023-0867-7

摘要： The effect of oxygen vacancies on the adsorption and activation of CO₂ on the surface of different phases of ZrO₂ is investigated by density functional theory (DFT) calculations. The calculations show that the oxygen vacancies contribute greatly to both the adsorption and activation of CO₂. The adsorption energy of CO₂ on the c-ZrO₂, t-ZrO₂ and, m-ZrO₂ surfaces is enhanced to 5, 4, and 3 folds with the help of oxygen vacancies, respectively. Moreover, the energy barrier of CO₂ dissociation on the defective surfaces of c-ZrO₂, t-ZrO₂, and m-ZrO₂ is reduced to 1/2, 1/4, and 1/5 of the perfect surface with the assistance of oxygen vacancies. Furthermore, the activation of CO₂ on the ZrO₂ surface where oxygen vacancies are present, and changes from an endothermic reaction to an exothermic reaction. This finding demonstrates that the presence of oxygen vacancies promotes the activation of CO₂ both kinetically and thermodynamically. These results could provide guidance for the high-efficient utilization of CO₂ at an atomic scale.

关键词： CO₂ activation oxygen vacancies ZrO₂ different phases

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Tuning porosity of coal-derived activated carbons for CO2 adsorption

《化学科学与工程前沿（英文）》 2022年第16卷第9期页码 1345-1354 doi: 10.1007/s11705-022-2155-1

摘要： A simple method was developed to tune the porosity of coal-derived activated carbons, which provided a model adsorbent system to investigate the volumetric CO₂ adsorption performance. Specifically, the method involved the variation of the activation temperature in a K₂CO₃ induced chemical activation process which could yield activated carbons with defined microporous (< 2 nm, including ultra-microporous < 1 nm) and meso-micro-porous structures. CO₂ adsorption isotherms revealed that the microporous activated carbon has the highest measured CO₂ adsorption capacity (6.0 mmol∙g^–1 at 0 °C and 4.1 mmol∙g^–1 at 25 °C), whilst ultra-microporous activated carbon with a high packing density exhibited the highest normalized capacity with respect to packing volume (1.8 mmol∙cm⁻³ at 0 °C and 1.3 mmol∙cm^–3 at 25 °C), which is significant. Both experimental correlation analysis and molecular dynamics simulation demonstrated that (i) volumetric CO₂ adsorption capacity is directly proportional to the ultra-micropore volume, and (ii) an increase in micropore sizes is beneficial to improve the volumetric capacity, but may lead a low CO₂ adsorption density and thus low pore space utilization efficiency. The adsorption experiments on the activated carbons established the criterion for designing CO₂ adsorbents with high volumetric adsorption capacity.

关键词： coal-derived activated carbons porosity CO₂ adsorption molecular dynamics

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Fabrication of coconut shell-derived porous carbons for CO adsorption application

《化学科学与工程前沿（英文）》 2023年第17卷第8期页码 1122-1130 doi: 10.1007/s11705-022-2292-6

摘要： Biomass-derived porous carbons have been considered as the most potential candidate for effective CO₂ adsorbent thanks to being widely-available precursor and having highly porous structure and stable chemical/physical features. However, the biomass-derived porous carbons still suffer from the poor optimization process in terms of the synthesis conditions. Herein, we have successfully fabricated coconut shell-derived porous carbon by a simple one-step synthesis process. The as-prepared carbon exhibits advanced textual activity together with well-designed micropore morphology and possesses oxygen-containing functional groups (reached 18.81 wt %) within the carbon matrix. Depending on the different activating temperatures (from 700 to 800 °C) and KOH/biomass mass ratios (from 0.3 to 1), the 750 °C and 0.5 mass ratio were found to be enabling the highest CO₂ capture performance. The optimal adsorbent was achieved a high CO₂ uptake capacity of 5.92 and 4.15 mmol·g⁻¹ at 0 and 25 °C (1 bar), respectively. More importantly, as-prepared carbon adsorbent exhibited moderate isosteric heat of adsorption and high CO₂/N₂ selectivity. The results were revealed not only the textural feature but also the surface functional groups critically determine the CO₂ capture performance, indicating coconut shell-derived porous carbon has a considerable potential as a solid-state adsorbent for the CO₂ capture.

关键词： porous carbons CO₂ adsorption KOH activation single step reaction biomass

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CO2sub> methanation and co-methanation of CO and CO2sub> over Mn-promoted Ni/Al2sub>O3sub> catalysts

Kechao Zhao,Zhenhua Li,Li Bian

《化学科学与工程前沿（英文）》 2016年第10卷第2期页码 273-280 doi: 10.1007/s11705-016-1563-5

摘要： A series of Mn-promoted 15 wt-% Ni/Al O catalysts were prepared by an incipient wetness impregnation method. The effect of the Mn content on the activity of the Ni/Al O catalysts for CO methanation and the co-methanation of CO and CO in a fixed-bed reactor was investigated. The catalysts were characterized by N physisorption, hydrogen temperature-programmed reduction and desorption, carbon dioxide temperature-programmed desorption, X-ray diffraction and high-resolution transmission electron microscopy. The presence of Mn increased the number of CO adsorption sites and inhibited Ni particle agglomeration due to improved Ni dispersion and weakened interactions between the nickel species and the support. The Mn-promoted 15 wt-% Ni/Al O catalysts had improved CO methanation activity especially at low temperatures (250 to 400 °C). The Mn content was varied from 0.86% to 2.54% and the best CO conversion was achieved with the 1.71Mn-Ni/Al O catalyst. The co-methanation tests on the 1.71Mn-Ni/Al O catalyst indicated that adding Mn markedly enhanced the CO methanation activity especially at low temperatures but it had little influence on the CO methanation performance. CO methanation was more sensitive to the reaction temperature and the space velocity than the CO methanation in the co-methanation process.

关键词： Mn promotion nickel catalysts CO₂ methanation co-methanation of CO and CO₂

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Detection of CO

Veselina Georgieva, Richard Retoux, Valerie Ruaux, Valentin Valtchev, Svetlana Mintova

《化学科学与工程前沿（英文）》 2018年第12卷第1期页码 94-102 doi: 10.1007/s11705-017-1692-5

摘要： Detection of oxygen and carbon dioxide is important in the field of chemical and biosensors for atmosphere and biosystem monitoring and fermentation processes. The present study reports on the preparation of zeolite films doped with iron nanoparticles for detection of CO and O in gas phase. Pure nanosized LTL type zeolite with monomodal particle size distribution loaded with iron (Fe-LTL) was prepared under hydrothermal condition from colloidal precursor suspensions. The zeolite was loaded with iron to different levels by ion exchange. The Fe-LTL suspensions were used for preparation of thin films on silicon wafers via spin coating method. The reduction of the iron in the zeolite films was carried out under H flow (50% H in Ar) at 300 °C. The presence of iron nanoparticles is proved by ultra-violet-visible spectroscopy. The properties of the films including surface roughness, thickness, porosity, and mechanical stability were studied. In addition, the loading and distribution of iron in the zeolite films were investigated. The Fe-LTL zeolite films were used to detect O and CO in a concentration dependent mode, followed by IR spectroscopy. The changes in the IR bands at 855 and 642 cm (Fe–O–H and Fe–O bending vibrations) and at 2363 and 2333 cm (CO asymmetric stretching) corresponding to the presence of O and CO , respectively, were evaluated. The response to O and CO was instant, which was attributed to great accessibility of the iron in the nanosized zeolite crystals. The saturation of the Fe-LTL films with CO and O at each concentration was reached within less than a minute. The Fe-LTL films detected both oxygen and carbon dioxide in contrast, to the pure LTL zeolite film.

关键词： zeolite films detection of CO₂ and O₂ adsorption

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以净零排放为目标的封存驱动型CO2sub>提高采收率方法 Article

刘月亮, 芮振华

《工程（英文）》 2022年第18卷第11期页码 79-87 doi: 10.1016/j.eng.2022.02.010

摘要：可通过驱油过程将CO2sub>封存在油藏地质体中，因此，CO2sub>驱油与封存被视为降低CO2sub>排放的重要手段之一。本研究提出了一种新型的CO2sub>提高采收率（EOR）方法，即封存驱动型CO2sub>提高采收率，其主要目标是通过在油藏中封存尽可能多的CO2sub>来实现CO结果表明，DME可提高CO2sub>在原油中的溶解度，有利于CO2sub>的溶解封存；可抑制因CO2sub>的抽提作用造成的原油轻质组分“逃逸&rdquo封存驱动型CO2sub> EOR方法在提高波及效率方面优于传统的CO2sub> EOR，尤其是在采油后期更为明显；同时，封存驱动型CO2sub> EOR比传统的此外，通过封存驱动型CO2sub> EOR封存的CO2sub>量远超采出原油燃烧产生的碳排放总量。

关键词： CO2sub> EOR CO2sub>净排放量二甲醚封存驱动型CO2sub> EOR CO2sub>封存

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Optimization of electrochemically synthesized Cu

Kasra Pirzadeh, Ali Asghar Ghoreyshi, Mostafa Rahimnejad, Maedeh Mohammadi

《化学科学与工程前沿（英文）》 2020年第14卷第2期页码 233-247 doi: 10.1007/s11705-019-1893-1

摘要： Cu (BTC) , a common type of metal organic framework (MOF), was synthesized through electrochemical route for CO capture and its separation from N . Taguchi method was employed for optimization of key parameters affecting the synthesis of Cu (BTC) . The results indicated that the optimum synthesis conditions with the highest CO selectivity can be obtained using 1 g of ligand, applied voltage of 25 V, synthesis time of 2 h, and electrode length of 3 cm. The single gas sorption capacity of the synthetized microstructure Cu (BTC) for CO (at 298 K and 1 bar) was a considerable value of 4.40 mmol·g . The isosteric heat of adsorption of both gases was calculated by inserting temperature-dependent form of Langmuir isotherm model in the Clausius-Clapeyron equation. The adsorption of CO /N binary mixture with a concentration ratio of 15/85 vol-% was also studied experimentally and the result was in a good agreement with the predicted value of IAST method. Moreover, Cu (BTC) showed no considerable loss in CO adsorption after six sequential cycles. In addition, artificial neural networks (ANNs) were also applied to predict the separation behavior of CO /N mixture by MOFs and the results revealed that ANNs could serve as an appropriate tool to predict the adsorptive selectivity of the binary gas mixture in the absence of experimental data.

关键词： Cu₃(BTC)₂ electrochemical synthesis CO₂ adsorption Taguchi optimization ANN modeling

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固体氧化物电解池共电解H2sub>O/CO2sub>研究进展

范慧,宋世栋,韩敏芳

《中国工程科学》 2013年第15卷第2期页码 107-112

摘要：本文介绍了固体氧化物电解池的结构特点及其用于H2O/CO2的共电解制备H2和CO的工作原理，综述了固体氧化物电解池的组成形式，以及单片电解池和电解池堆用于H2O/CO2共电解反应的国内外研究进展，并阐述了提高固体氧化物电解池共电解效率所亟需解决的问题

关键词：固体氧化物电解池 H2sub>O/CO2sub>共电解合成气电解效率水电解

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CO, N, and CO/N mixed gas injection for enhanced shale gas recovery and CO geological storage

《能源前沿（英文）》 2023年第17卷第3期页码 428-445 doi: 10.1007/s11708-023-0865-9

摘要： In this work, using fractured shale cores, isothermal adsorption experiments and core flooding tests were conducted to investigate the performance of injecting different gases to enhance shale gas recovery and CO₂ geological storage efficiency under real reservoir conditions. The adsorption process of shale to different gases was in agreement with the extended-Langmuir model, and the adsorption capacity of CO₂ was the largest, followed by CH_4, and that of N₂ was the smallest of the three pure gases. In addition, when the CO₂ concentration in the mixed gas exceeded 50%, the adsorption capacity of the mixed gas was greater than that of CH₄, and had a strong competitive adsorption effect. For the core flooding tests, pure gas injection showed that the breakthrough time of CO₂ was longer than that of N₂, and the CH₄ recovery factor at the breakthrough time (

R C H 4

) was also higher than that of N₂. The

R C H 4

of CO₂ gas injection was approximately 44.09%, while the

R C H 4

of N₂ was only 31.63%. For CO₂/N₂ mixed gas injection, with the increase of CO₂ concentration, the

R C H 4

increased, and the

R C H 4

for mixed gas CO₂/N₂ = 8:2 was close to that of pure CO₂, about 40.24%. Moreover, the breakthrough time of N₂ in mixed gas was not much different from that when pure N₂ was injected, while the breakthrough time of CO₂ was prolonged, which indicated that with the increase of N₂ concentration in the mixed gas, the breakthrough time of CO₂ could be extended. Furthermore, an abnormal surge of N₂ concentration in the produced gas was observed after N₂ breakthrough. In regards to CO₂ storage efficiency (

S s t o r a g e - C O 2

), as the CO₂ concentration increased,

S s t o r a g e - C O 2

also increased. The

S s t o r a g e - C O 2

of the pure CO₂ gas injection was about 35.96%, while for mixed gas CO₂/N₂ = 8:2,

S s t o r a g e - C O 2

was about 32.28%.

关键词： shale gas gas injection competitive adsorption enhanced shale gas recovery CO₂ geological storage

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Frontier science and challenges on offshore carbon storage

《环境科学与工程前沿（英文）》 2023年第17卷第7期 doi: 10.1007/s11783-023-1680-6

摘要：

● The main direct seal up carbon options and challenges are reviewed.

关键词： Offshore carbon storage Direct CO₂ injection CO₂-CH₄ replacement CO₂-EOR CCS hubs CO₂ transport

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Integrated adsorption and absorption process for post-combustion CO

Gongkui Xiao, Penny Xiao, Andrew Hoadley, Paul Webley

《化学科学与工程前沿（英文）》 2021年第15卷第3期页码 483-492 doi: 10.1007/s11705-020-1964-3

摘要： This study explored the feasibility of integrating an adsorption and solvent scrubbing process for post-combustion CO capture from a coal-fired power plant. This integrated process has two stages: the first is a vacuum swing adsorption (VSA) process using activated carbon as the adsorbent, and the second stage is a solvent scrubber/stripper system using monoethanolamine (30 wt-%) as the solvent. The results showed that the adsorption process could enrich CO in the flue gas from 12 to 50 mol-% with a CO recovery of >90%, and the concentrated CO stream fed to the solvent scrubber had a significantly lower volumetric flowrate. The increased CO concentration and reduced feed flow to the absorption section resulted in significant reduction in the diameter of the solvent absorber, bringing the size of the absorber from uneconomically large to readily achievable domain. In addition, the VSA process could also remove most of the oxygen initially existed in the feed gas, alleviating the downstream corrosion and degradation problems in the absorption section. The findings in this work will reduce the technical risks associated with the state-of-the art solvent absorption technology for CO capture and thus accelerate the deployment of such technologies to reduce carbon emissions.

关键词： vacuum swing adsorption monoethanolamine post-combustion CO₂ capture integrated process

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Reduction potential of the energy penalty for CO capture in CCS

《能源前沿（英文）》 2023年第17卷第3期页码 390-399 doi: 10.1007/s11708-023-0864-x

摘要： CO₂ capture and storage (CCS) has been acknowledged as an essential part of a portfolio of technologies that are required to achieve cost-effective long-term CO₂ mitigation. However, the development progress of CCS technologies is far behind the targets set by roadmaps, and engineering practices do not lead to commercial deployment. One of the crucial reasons for this delay lies in the unaffordable penalty caused by CO₂ capture, even though the technology has been commonly recognized as achievable. From the aspects of separation and capture technology innovation, the potential and promising direction for solving this problem were analyzed, and correspondingly, the possible path for deployment of CCS in China was discussed. Under the carbon neutral target recently proposed by the Chinese government, the role of CCS and the key milestones for deployment were indicated.

关键词： CO₂ capture and storage (CCS) CO₂ separation energy penalty

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Al2sub>O3sub> and CeO2sub>-promoted MgO sorbents for CO2sub> capture at moderate

Huimei Yu, Xiaoxing Wang, Zhu Shu, Mamoru Fujii, Chunshan Song

《化学科学与工程前沿（英文）》 2018年第12卷第1期页码 83-93 doi: 10.1007/s11705-017-1691-6

摘要： A series of Al O and CeO modified MgO sorbents was prepared and studied for CO sorption at moderate temperatures. The CO sorption capacity of MgO was enhanced with the addition of either Al O or CeO . Over Al O -MgO sorbents, the best capacity of 24.6 mg-CO /g-sorbent was attained at 100 °C, which was 61% higher than that of MgO (15.3 mg-CO /g-sorbent). The highest capacity of 35.3 mg-CO /g-sorbent was obtained over the CeO -MgO sorbents at the optimal temperature of 200 °C. Combining with the characterization results, we conclude that the promotion effect on CO sorption with the addition of Al O and CeO can be attributed to the increased surface area with reduced MgO crystallite size. Moreover, the addition of CeO increased the basicity of MgO phase, resulting in more increase in the CO capacity than Al O promoter. Both the Al O -MgO and CeO -MgO sorbents exhibited better cyclic stability than MgO over the course of fifteen CO sorption-desorption cycles. Compared to Al O , CeO is more effective for promoting the CO capacity of MgO. To enhance the CO capacity of MgO sorbent, increasing the basicity is more effective than the increase in the surface area.

关键词： CO₂ capture MgO sorbents Al₂O₃ CeO₂ flue gas

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ZnFe2sub>O4sub> deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO2sub> in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

《化学科学与工程前沿（英文）》 2017年第11卷第2期页码 197-204 doi: 10.1007/s11705-016-1606-y

摘要： ZnFe O -BiOCl composites were prepared by both hydrothermal and direct precipitation processes and the structures and properties of the samples were characterized by various instrumental techniques. The samples were then used as catalysts for the photocatalytic reduction of CO in cyclohexanol under ultraviolet irradiation to give cyclohexanone (CH) and cyclohexyl formate (CF). The photocatalytic CO reduction activities over the hydrothermally prepared ZnFe O -BiOCl composites were higher than those over the directly-precipitated composites. This is because compared to the direct-precipitation sample, the ZnFe O nanoparticles in the hydrothermal sample were smaller and more uniformly distributed on the surface of BiOCl and so more heterojunctions were formed. Higher CF and CH yields were obtained for the pure BiOCl and BiOCl composite samples with more exposed (001) facets than for the samples with more exposed (010) facets. This is due to the higher density of oxygen atoms in the exposed (001) facets, which creates more oxygen vacancies, and thereby improves the separation efficiency of the electron-hole pairs. More importantly, irradiation of the (001) facets with ultraviolet light produces photo-generated electrons which is helpful for the reduction of CO to ·CO . The mechanism for the photocatalytic reduction of CO in cyclohexanol over ZnFe O -BiOCl composites with exposed (001) facets involves electron transfer and carbon radical formation.

关键词： reduction of CO₂ cyclohexanol ZnFe₂O₄ deposited BiOCl facet composite photocatalyst

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Efficient CO

Yanxia Wang, Xiude Hu, Tuo Guo, Jian Hao, Chongdian Si, Qingjie Guo

《化学科学与工程前沿（英文）》 2021年第15卷第3期页码 493-504 doi: 10.1007/s11705-020-1967-0

摘要： In this work, nitrogen-doped porous carbons (NACs) were fabricated as an adsorbent by urea modification and KOH activation. The CO adsorption mechanism for the NACs was then explored. The NACs are found to present a large specific surface area (1920.72–3078.99 m ·g ) and high micropore percentage (61.60%–76.23%). Under a pressure of 1 bar, sample NAC-650-650 shows the highest CO adsorption capacity up to 5.96 and 3.92 mmol·g at 0 and 25 °C, respectively. In addition, the CO /N selectivity of NAC-650-650 is 79.93, much higher than the value of 49.77 obtained for the nonnitrogen-doped carbon AC-650-650. The CO adsorption capacity of the NAC-650-650 sample maintains over 97% after ten cycles. Analysis of the results show that the CO capacity of the NACs has a linear correlation ( = 0.9633) with the cumulative pore volume for a pore size less than 1.02 nm. The presence of nitrogen and oxygen enhances the CO /N selectivity, and pyrrole-N and hydroxy groups contribute more to the CO adsorption. Fourier transform infrared spectra analysis indicates that CO is adsorbed onto the NACs as a gas. Furthermore, the physical adsorption mechanism is confirmed by adsorption kinetic models and the isosteric heat, and it is found to be controlled by CO diffusion. The CO adsorption kinetics for NACs at room temperature and in pure CO is in accordance with the pseudo-first-order model and Avramís fractional-order kinetic model.

关键词： porous carbon CO₂ adsorption nitrogen-doped adsorption mechanism kinetics