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Co anchored on porphyrinic triazine-based frameworks with excellent biocompatibility for conversion ofCO in H-mediated microbial electrosynthesis

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1761-1771 doi: 10.1007/s11705-022-2195-6

摘要： Microbial electrosynthesis is a promising alternative to directly convert CO2 into long-chain compounds by coupling inorganic electrocatalysis with biosynthetic systems. However, problems arose that the conventional electrocatalysts for hydrogen evolution may produce extensive by-products of reactive oxygen species and cause severe metal leaching, both of which induce strong toxicity toward microorganisms. Moreover, poor stability of electrocatalysts cannot be qualified for long-term operation. These problems may result in poor biocompatibility between electrocatalysts and microorganisms. To solve the bottleneck problem, Co anchored on porphyrinic triazine-based frameworks was synthesized as the electrocatalyst for hydrogen evolution and further coupled with Cupriavidus necator H16. It showed high selectivity for a four-electron pathway of oxygen reduction reaction and low production of reactive oxygen species, owing to the synergistic effect of Co–Nx modulating the charge distribution and adsorption energy of intermediates. Additionally, low metal leaching and excellent stability were observed, which may be attributed to low content of Co and the stabilizing effect of metalloporphyrins. Hence, the electrocatalyst exhibited excellent biocompatibility. Finally, the microbial electrosynthesis system equipped with the electrocatalyst successfully converted CO2 to poly-β-hydroxybutyrate. This work drew up a novel strategy for enhancing the biocompatibility of electrocatalysts in microbial electrosynthesis system.

关键词： microbial electrosynthesis     hydrogen evolution reaction     metalloporphyrins     biocompatibility     CO2 conversion    

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CO<sub>2sub> methanation and co-methanation of CO and CO<sub>2sub> over Mn-promoted Ni/Al<sub>2sub>O<sub>3sub> 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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以净零排放为目标的封存驱动型CO<sub>2sub>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CO<sub>2sub>封存在油藏地质体中，因此，CO<sub>2sub>驱油与封存被视为降低CO<sub>2sub>排放的重要手段之一。本研究提出了一种新型的CO<sub>2sub>提高采收率（EOR）方法，即封存驱动型CO<sub>2sub>提高采收率，其主要目标是通过在油藏中封存尽可能多的CO<sub>2sub>来实现CO结果表明，DME可提高CO<sub>2sub>在原油中的溶解度，有利于CO<sub>2sub>的溶解封存；可抑制因CO<sub>2sub>的抽提作用造成的原油轻质组分“逃逸&rdquo封存驱动型CO<sub>2sub> EOR方法在提高波及效率方面优于传统的CO<sub>2sub> EOR，尤其是在采油后期更为明显；同时，封存驱动型CO<sub>2sub> EOR比传统的此外，通过封存驱动型CO<sub>2sub> EOR封存的CO<sub>2sub>量远超采出原油燃烧产生的碳排放总量。

关键词： CO<sub>2sub> EOR     CO<sub>2sub>净排放量     二甲醚     封存驱动型CO<sub>2sub> EOR     CO<sub>2sub>封存    

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Conversion of CO into CO by high active and stable PdNi nanoparticles supported on a metal-organic framework

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1139-1148 doi: 10.1007/s11705-021-2111-5

摘要： The solubility of Pd(NO3)2 in water is moderate whereas it is completely soluble in diluted HNO3 solution. Pd/MIL-101(Cr) and Pd/MIL-101-NH2(Cr) were synthesized by aqueous solution of Pd(NO3)2 and Pd(NO3)2 solution in dilute HNO3 and used for CO oxidation reaction. The catalysts synthesized with Pd(NO3)2 solution in dilute HNO3 showed lower activity. The aqueous solution of Pd(NO3)2 was used for synthesis of mono-metal Ni, Pd and bimetallic PdNi nanoparticles with various molar ratios supported on MOF. Pd70Ni30/MIL-101(Cr) catalyst showed higher activity than monometallic counterparts and Pd+ Ni physical mixture due to the strong synergistic effect of PdNi nanoparticles, high distribution of PdNi nanoparticles, and lower dissociation and desorption barriers. Comparison of the catalysts synthesized by MIL-101(Cr) and MIL-101-NH2(Cr) as the supports of metals showed that Pd/MIL-101-NH2(Cr) outperforms Pd/MIL-101-(Cr) because of the higher electron density of Pd resulting from the electron donor ability of the NH2 functional group. However, the same activities were observed for Pd70Ni30/MIL-101(Cr) and Pd70Ni30/MIL-101-NH2(Cr), which is due to a less uniform distribution of Pd nanoparticles in Pd70Ni30/MIL-101-NH2(Cr) originated from amorphization of MIL-101-NH2(Cr) structure during the reduction process. In contrast, Pd70Ni30/MIL-101(Cr) revealed the stable structure and activity during reduction and CO oxidation for a long time.

关键词： CO oxidation     heterogeneous catalysis     metal-organic framework     NH2 functional group     PdNi    

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固体氧化物电解池共电解H<sub>2sub>O/CO<sub>2sub>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     H<sub>2sub>O/CO<sub>2sub>共电解     合成气     电解效率     水电解    

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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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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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Al<sub>2sub>O<sub>3sub> and CeO<sub>2sub>-promoted MgO sorbents for CO<sub>2sub> 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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ZnFe<sub>2sub>O<sub>4sub> deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO<sub>2sub> 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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太阳能技术对我国未来减排CO<sub>2sub> 的贡献

赵玉文

《中国工程科学》 2003年 第5卷 第4期   页码 38-40

摘要：

在“我国后续能源发展战略研究”基础上对太阳能技术在我国未来减排CO<sub>2sub>中的作用进行了估计，结果表明，在2010年后太阳能技术对CO<sub>2sub

关键词： 太阳能，CO2减排    

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Boosting the direct conversion of NHHCO electrolyte to syngas on Ag/Zn zeolitic imidazolate framework

《化学科学与工程前沿（英文）》 2023年 第17卷 第9期   页码 1196-1207 doi: 10.1007/s11705-022-2289-1

摘要： The electrochemical reduction of NH4HCO3 to syngas can bypass the high energy consumption of high-purity CO2 release and compression after the ammonia-based CO2 capture process. This technology has broad prospects in industrial applications and carbon neutrality. A zeolitic imidazolate framework-8 precursor was introduced with different Ag contents via colloid chemical synthesis. This material was carbonized at 1000 °C to obtain AgZn zeolitic imidazolate framework derived nitrogen carbon catalysts, which were used for the first time for boosting the direct conversion of NH4HCO3 electrolyte to syngas. The AgZn zeolitic imidazolate framework derived nitrogen carbon catalyst with a Ag/Zn ratio of 0.5:1 achieved the highest CO Faradaic efficiency of 52.0% with a current density of 1.15 mA·cm–2 at –0.5 V, a H2/CO ratio of 1–2 (–0.5 to –0.7 V), and a stable catalytic activity of more than 6 h. Its activity is comparable to that of the CO2-saturated NH4HCO3 electrolyte. The highly discrete Ag-Nx and Zn-Nx nodes may have combined catalytic effects in the catalysts synthesized by appropriate Ag doping and sufficient carbonization. These nodes could increase active sites of catalysts, which is conducive to the transport and adsorption of reactant CO2 and the stability of *COOH intermediate, thus can improve the selectivity and catalytic activity of CO.

关键词： Ag catalyst     zeolitic imidazolate framework     CO2 electroreduction     ammonium bicarbonate electrolyte     syngas    

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Plasma-catalysis: Is it just a question of scale?

J. Christopher Whitehead

《化学科学与工程前沿（英文）》 2019年 第13卷 第2期   页码 264-273 doi: 10.1007/s11705-019-1794-3

摘要： The issues of describing and understanding the changes in performance that result when a catalyst is placed into plasma are discussed. The different chemical and physical interactions that result and how their combination might produce beneficial results for the plasma-catalytic processing of different gas streams are outlined with particular emphasis being placed on the different range of spatial and temporal scales that must be considered both in experiment and modelling. The focus is on non-thermal plasma where the lack of thermal equilibrium creates a range of temperature scales that must be considered. This contributes in part to a wide range of inhomogeneity in different properties such as species concentrations and electric fields that must be determined experimentally by methods and be incorporated into modelling. It is concluded that plasma-catalysis is best regarded as conventional catalysis perturbed by the presence of a discharge, which modifies its operating conditions, properties and outcomes often in a very localised way. The sometimes used description “plasma-activated catalysis” is an apt one.

关键词： plasma catalysis     plasma-activated catalysis     non-thermal plasma     CO2 conversion    

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A CO and CO

Guoxing Chen, Marc Widenmeyer, Binjie Tang, Louise Kaeswurm, Ling Wang, Armin Feldhoff, Anke Weidenkaff

《化学科学与工程前沿（英文）》 2020年 第14卷 第3期   页码 405-414 doi: 10.1007/s11705-019-1886-0

摘要： A series of novel dense mixed conducting ceramic membranes based on K NiF -type (La Ca ) (Ni Cu )O was successfully prepared through a sol-gel route. Their chemical compatibility, oxygen permeability, CO and CO tolerance, and long-term CO resistance regarding phase composition and crystal structure at different atmospheres were studied. The results show that higher Ca contents in the material lead to the formation of CaCO . A constant oxygen permeation flux of about 0.63 mL·min ·cm at 1173 K through a 0.65 mm thick membrane was measured for (La Ca ) (Ni Cu )O , using either helium or pure CO as sweep gas. Steady oxygen fluxes with no sign of deterioration of this membrane were observed with increasing CO concentration. The membrane showed excellent chemical stability towards CO for more than 1360 h and phase stability in presence of CO for 4 h at high temperature. In addition, this membrane did not deteriorate in a high-energy CO plasma. The present work demonstrates that this (La Ca ) (Ni Cu )O membrane is a promising chemically robust candidate for oxygen separation applications.

关键词： K2NiF4 structure     oxygen permeation membrane     CO2 and CO resistances     CO2 plasma resistance     long-term robustness    

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基于实时CT扫描技术的CO<sub>2sub>和N<sub>2sub>交替注入条件下煤吸附膨胀和解吸收缩规律研究 Article

张广磊, P.G. Ranjith, Herbert E. Huppert

《工程（英文）》 2022年 第18卷 第11期   页码 88-95 doi: 10.1016/j.eng.2022.03.010

摘要：

深部煤层是分布最广泛的适宜二氧化碳（CO<sub>2sub>）地质封存的地层之一，且通常位于大型CO<sub>2sub>排放源附近。将CO<sub>2sub>注入到煤层中具有巨大的CO<sub>2sub>封存潜力，同时可以提高煤层气的采收率（CO<sub>2sub>-ECBM）。然而，目前CO<sub>2sub>-ECBM先导实验仍存在技术问题需要解决，即CO<sub>2sub>的注入会引起煤层渗透率降低进而影响长期注入能力。本文采用原位同步辐射X射线显微CT扫描技术，首次在原位条件下直接证明了注入氮气（N<sub>2sub>）可以置换解吸CO<sub>2sub>并减小因CO<sub>2sub>吸附引起的煤基质膨胀研究结果表明，煤层中注入经过简单处理的烟道气（主要成分为N<sub>2sub>和CO<sub>2sub>），是技术上可行的CO<sub>2sub>-ECBM 替代方案。

关键词： CCS     CO<sub>2sub>-ECBM     碳中和     X 射线成像     煤渗透率    

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Nickel(II) ion-intercalated MXene membranes for enhanced H<sub>2sub>/CO<sub>2sub> separation

Yiyi Fan, Jinyong Li, Saidi Wang, Xiuxia Meng, Yun Jin, Naitao Yang, Bo Meng, Jiaquan Li, Shaomin Liu

《化学科学与工程前沿（英文）》 2021年 第15卷 第4期   页码 882-891 doi: 10.1007/s11705-020-1990-1

摘要： Hydrogen fuel has been embraced as a potential long-term solution to the growing demand for clean energy. A membrane-assisted separation is promising in producing high-purity H . Molecular sieving membranes (MSMs) are endowed with high gas selectivity and permeability because their well-defined micropores can facilitate molecular exclusion, diffusion, and adsorption. In this work, MXene nanosheets intercalated with Ni were assembled to form an MSM supported on Al O hollow fiber via a vacuum-assisted filtration and drying process. The prepared membranes showed excellent H /CO mixture separation performance at room temperature. Separation factor reached 615 with a hydrogen permeance of 8.35 × 10 mol·m ·s ·Pa . Compared with the original Ti C T /Al O hollow fiber membranes, the permeation of hydrogen through the Ni -Ti C T /Al O membrane was considerably increased, stemming from the strong interaction between the negatively charged MXene nanosheets and Ni . The interlayer spacing of MSMs was tuned by Ni . During 200-hour testing, the resultant membrane maintained an excellent gas separation without any substantial performance decline. Our results indicate that the Ni tailored Ti C T /Al O hollow fiber membranes can inspire promising industrial applications.

关键词： MXene     H2/CO2 separation     nickel ions     hollow fiber    

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标题 作者 时间 类型 操作

Co anchored on porphyrinic triazine-based frameworks with excellent biocompatibility for conversion ofCO in H-mediated microbial electrosynthesis

期刊论文

CO<sub>2sub> methanation and co-methanation of CO and CO<sub>2sub> over Mn-promoted Ni/Al<sub>2sub>O<sub>3sub> catalysts

Kechao Zhao,Zhenhua Li,Li Bian

期刊论文

以净零排放为目标的封存驱动型CO<sub>2sub>提高采收率方法

刘月亮, 芮振华

期刊论文

Conversion of CO into CO by high active and stable PdNi nanoparticles supported on a metal-organic framework

期刊论文

固体氧化物电解池共电解H<sub>2sub>O/CO<sub>2sub>研究进展

范慧,宋世栋,韩敏芳

期刊论文

Frontier science and challenges on offshore carbon storage

期刊论文

Reduction potential of the energy penalty for CO capture in CCS

期刊论文

Al<sub>2sub>O<sub>3sub> and CeO<sub>2sub>-promoted MgO sorbents for CO<sub>2sub> capture at moderate

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

期刊论文

ZnFe<sub>2sub>O<sub>4sub> deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO<sub>2sub> in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

期刊论文

太阳能技术对我国未来减排CO<sub>2sub> 的贡献

赵玉文

期刊论文

Boosting the direct conversion of NHHCO electrolyte to syngas on Ag/Zn zeolitic imidazolate framework

期刊论文

Plasma-catalysis: Is it just a question of scale?

J. Christopher Whitehead

期刊论文

A CO and CO

Guoxing Chen, Marc Widenmeyer, Binjie Tang, Louise Kaeswurm, Ling Wang, Armin Feldhoff, Anke Weidenkaff

期刊论文

基于实时CT扫描技术的CO<sub>2sub>和N<sub>2sub>交替注入条件下煤吸附膨胀和解吸收缩规律研究

张广磊, P.G. Ranjith, Herbert E. Huppert

期刊论文

Nickel(II) ion-intercalated MXene membranes for enhanced H<sub>2sub>/CO<sub>2sub> separation

Yiyi Fan, Jinyong Li, Saidi Wang, Xiuxia Meng, Yun Jin, Naitao Yang, Bo Meng, Jiaquan Li, Shaomin Liu

期刊论文