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钾/锰助剂对氮掺杂碳纳米管负载铁基催化剂在CO<sub>2sub>加氢过程中的影响研究 Article

Praewpilin Kangvansura, Ly May Chew, Chanapa Kongmark, Phatchada Santawaja, Holger Ruland, Wei Xia, Hans Schulz, Attera Worayingyong, Martin Muhler

《工程(英文)》 2017年 第3卷 第3期   页码 385-392 doi: 10.1016/J.ENG.2017.03.013

摘要:

氮掺杂碳纳米管(NCNTs) 作为载体负载铁(Fe) 纳米颗粒,可应用于CO<sub>2sub>多相催化加氢反应(633 K和25 bar)。当将钾(K) 和锰(Mn) 作为助催化剂时,Fe/NCNT 展现出优异的CO<sub>2sub> 加氢性能,在体积空速(GHSV) 为3.1 L·(g·h)&ndash通过探针反应NH<sub>3sub> 的催化分解来表征助催化剂效应。当K 和Mn 作为助催化剂时,Fe/NCNT 具有最好的催化活性。

关键词: CO<sub>2sub> 加氢     铁基催化剂     n 型碳纳米管     Mn 助剂     K 助剂    

Rh<sub>2sub>O<sub>3sub>/hexagonal CePO<sub>4sub> nanocatalysts for N<sub>2sub>O decomposition

Huan Liu, Zhen Ma

《化学科学与工程前沿(英文)》 2017年 第11卷 第4期   页码 586-593 doi: 10.1007/s11705-017-1659-6

摘要: Hexagonal CePO nanorods were prepared by a precipitation method and hexagonal CePO nanowires were prepared by hydrothermal synthesis at 150 °C. Rh(NO ) was then used as a precursor for the impregnation of Rh O onto these CePO materials. The Rh O supported on the CePO nanowires was much more active for the catalytic decomposition of N O than the Rh O supported on CePO nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO , O , H O or O /H O) on the N O decomposition was also investigated. The samples were characterized by N adsorption-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-programmed reduction, oxygen temperature-programmed desorption, and CO temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.

关键词: Rh2O3     CePO4     N2O decomposition    

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    

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    

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    

The stabilization effect of Al<sub>2sub>O<sub>3sub> on unconventional Pb/SiO<sub>2sub> catalyst

《化学科学与工程前沿(英文)》 2023年 第17卷 第10期   页码 1423-1429 doi: 10.1007/s11705-023-2315-y

摘要: Similar to Sn, Pb located at the same group (IVA) in the periodic table of elements, can also catalyze propane dehydrogenation to propene, while a fast deactivation can be observed. To enhance the stability, the traditional carrier Al2O3 with a small amount, was introduced into Pb/SiO2 catalyst in this study. It has been proved that Al2O3 can inhibit the reduction of PbO, and weaken the agglomeration and loss of Pb species due to its enhanced interaction with Pb species. As a result, 3Al15Pb/SiO2 catalyst exhibits a much higher stability up to more than 150 h. In addition, a simple schematic diagram of the change of surface species on the catalyst surface after Al2O3 addition was also proposed.

关键词: Pb/SiO2     Al2O3     propane dehydrogenation     propene     stability    

Cu-doped Bi/Bi<sub>2sub>WO<sub>6sub> catalysts for efficient N<sub>2sub> fixation by photocatalysis

《化学科学与工程前沿(英文)》 2023年 第17卷 第10期   页码 1412-1422 doi: 10.1007/s11705-023-2312-1

摘要: In this paper, Cu-doped Bi2WO6 was synthesized via a solvothermal method and applied it in photocatalytic N2 immobilization. Characterization results showed the presence of a small amount of metallic Bi in the photocatalyst, indicating that the synthesized photocatalyst is actually Bi/Cu-Bi2WO6 composite. The doped Cu had a valence state of +2 and most likely substituted the position of Bi3+. The introduced Cu did not affect the metallic Bi content, but mainly influenced the energy band structure of Bi2WO6. The band gap was slightly narrowed, the conduction band was elevated, and the work function was reduced. The reduced work function improved the transfer and separation of charge carriers, which mainly caused the increased photoactivity. The optimized NH3 generation rates of Bi/Cu-Bi2WO6 reached 624 and 243 μmol·L–1·g–1·h–1 under simulated solar and visible light, and these values were approximately 2.8 and 5.9 times higher those of Bi/Bi2WO6, respectively. This research provides a method for improving the photocatalytic N2 fixation and may provide more information on the design and preparation of heteroatom-doped semiconductor photocatalysts for N2-to-NH3 conversion.

关键词: Bi2WO6     Cu doping     work function     photocatalytic N2 fixation     charge separation    

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    

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    

含稀释剂的Al-Cr<sub>2sub>O<sub>3sub>体系燃烧合成反应热力学分析与反应模型

张衍诚,潘冶,张传

《中国工程科学》 2004年 第6卷 第6期   页码 63-67

摘要:

对含稀释剂Al203和Cr<sub>2</sub>0<sub>3</sub>的Al-Cr<sub>2</sub>0<sub>3</sub>体系燃烧合成反应进行了热力学计算与分析,讨论了起始反应温度T<sub>0</sub>、稀释剂Al<sub>2</sub>O<sub>3</sub>和Cr<sub>2</sub>O<sub>3</sub>的含量对绝热反应温度7^的影响,并得出T<sub>0</sub>与T<sub>ad</sub>在特定温度段上的近似线性关系以及该关系在指导材料成分设计上的应用;揭示了反应驱动力—&mdash

关键词: 金属陶瓷     燃烧合成     Al-Cr203体系     热力学     反应模型    

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    

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    

Interfacial charge transfer and photocatalytic activity in a reverse designed BiO/TiO core-shell

《能源前沿(英文)》 2021年 第15卷 第3期   页码 732-743 doi: 10.1007/s11708-021-0772-x

摘要: In this study, the electronic and photocatalytic properties of core-shell heterojunctions photocatalysts with reversible configuration of TiO2 and Bi2O3 layers were studied. The core-shell nanostructure, obtained by efficient control of the sol-gel polymerization and impregnation method of variable precursors of semiconductors, makes it possible to study selectively the role of the interfacial charge transfer in each configuration. The morphological, optical, and chemical composition of the core-shell nanostructures were characterized by high-resolution transmission electron microscopy, UV-visible spectroscopy and X-ray photoelectron spectroscopy. The results show the formation of homogenous TiO2 anatase and Bi2O3 layers with a thickness of around 10 and 8 nm, respectively. The interfacial charge carrier dynamic was tracked using time resolved microwave conductivity and transition photocurrent density. The charge transfer, their density, and lifetime were found to rely on the layout layers in the core-shell nanostructure. In optimal core-shell design, Bi2O3 collects holes from TiO2, leaving electrons free to react and increase by 5 times the photocatalytic efficiency toward H2 generation. This study provides new insight into the importance of the design and elaboration of optimal heterojunction based on the photocatalyst system to improve the photocatalytic activity.

关键词: photocatalysis     core-shell     heterojunction     H2     TiO2     Bi2O3    

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)。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。其次,N<sub>2sub>的存在可以使煤层保持较高的渗透率,实现长期CO<sub>2sub>注入封存和煤层气增产。

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

In-MOF-derived In<sub>2sub>S<sub>3sub>/Bi<sub>2sub>S<sub>3sub> heterojunction for enhanced photocatalytic

《能源前沿(英文)》 2023年 第17卷 第5期   页码 654-663 doi: 10.1007/s11708-023-0885-5

摘要: Transition metal sulfides are commonly studied as photocatalysts for water splitting in solar-to-fuel conversion. However, the effectiveness of these photocatalysts is limited by the recombination and restricted light absorption capacity of carriers. In this paper, a broad spectrum responsive In2S3/Bi2S3 heterojunction is constructed by in-situ integrating Bi2S3 with the In2S3, derived from an In-MOF precursor, via the high-temperature sulfidation and solvothermal methods. Benefiting from the synergistic effect of wide-spectrum response, effective charge separation and transfer, and strong heterogeneous interfacial contacts, the In2S3/Bi2S3 heterojunction demonstrates a rate of 0.71 mmol/(g∙h), which is 2.2 and 1.7 times as much as those of In2S3 (0.32 mmol/(g∙h) and Bi2S3 (0.41 mmol/(g∙h)), respectively. This paper provides a novel idea for rationally designing innovative heterojunction photocatalysts of transition metal sulfides for photocatalytic hydrogen production.

关键词: photocatalytic hydrogen production     wide-spectrum response     metal sulfides     MOFs derivative     heterogeneous interfacial contact    

标题 作者 时间 类型 操作

钾/锰助剂对氮掺杂碳纳米管负载铁基催化剂在CO<sub>2sub>加氢过程中的影响研究

Praewpilin Kangvansura, Ly May Chew, Chanapa Kongmark, Phatchada Santawaja, Holger Ruland, Wei Xia, Hans Schulz, Attera Worayingyong, Martin Muhler

期刊论文

Rh<sub>2sub>O<sub>3sub>/hexagonal CePO<sub>4sub> nanocatalysts for N<sub>2sub>O decomposition

Huan Liu, Zhen Ma

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

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

The stabilization effect of Al<sub>2sub>O<sub>3sub> on unconventional Pb/SiO<sub>2sub> catalyst

期刊论文

Cu-doped Bi/Bi<sub>2sub>WO<sub>6sub> catalysts for efficient N<sub>2sub> fixation by photocatalysis

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

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

含稀释剂的Al-Cr<sub>2sub>O<sub>3sub>体系燃烧合成反应热力学分析与反应模型

张衍诚,潘冶,张传

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

Frontier science and challenges on offshore carbon storage

期刊论文

Interfacial charge transfer and photocatalytic activity in a reverse designed BiO/TiO core-shell

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

In-MOF-derived In<sub>2sub>S<sub>3sub>/Bi<sub>2sub>S<sub>3sub> heterojunction for enhanced photocatalytic

期刊论文