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固体氧化物电解电解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:

固体氧化物电解池(SOEC)作为一种新的能源利用方式,可以将电能转化为化学能,具有高效、洁净、环保等优点。本文介绍了固体氧化物电解池的结构特点及其用于H2O/CO2电解制备H2CO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电解效率所亟需解决的问题

关键词: 固体氧化物电解    H<sub>2sub>O/CO<sub>2sub>电解     合成气     电解效率     电解    

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    

电解用Fe-Ni-Co-Al<sub>2sub>O<sub>3sub>金属陶瓷惰性阳极

邱竹贤,石忠宁,徐君莉

《中国工程科学》 2004年 第6卷 第8期   页码 35-39

摘要:

研制了一种新型铝电解金属陶瓷惰性阳极,阳极基体由Fe-Ni-CoAl<sub>2sub>O<sub>3sub>构成。在石墨坩埚中,960℃温度下,电解质中的氧化铝质量分数为6.0%,摩尔比为2.6;阳极电流密度为1.0 A/cm2,阳极尺寸大小为120 mm×80 mm×15 mm,石墨阴极尺寸大小为120 mm×40 mm×20 mm,通入的直流电为100~300 A,电解时间各为10 h;实验所得的电解铝产品纯度达到98%以上,杂质主要为Fe,Ni,Co电解后的阳极外观尺寸无明显变化,阳极气体中氧气质量分数达到98%~99%。阳极的反电动势为2.45 V,比理论分解电压仅高出0.25 V证明该阳极为惰性阳极,在电解槽中进行的是Al<sub>2sub>O<sub>3sub>的分解反应。

关键词: 电解     惰性阳极     反电动势    

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    

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    

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    

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    

H<sub>2sub> 对Pt-Ba-Ce /γ-Al<sub>2sub>O<sub>3sub> 催化剂NO<sub>xsub> 存储和还原机理的影响研究 Article

王攀, 裔静, 孙川, 罗鹏, 雷利利

《工程(英文)》 2019年 第5卷 第3期   页码 568-575 doi: 10.1016/j.eng.2019.02.005

摘要:

本研究采用浸渍法制备了Pt-Ba-Ce/γ-Al<sub>2sub>O<sub>3sub>催化剂,利用实验评价了H<sub>2sub> 对NSR(NO<sub>xsub> storage and reduction)催化剂存储和还原机理的影响,并采用综合表征技术研究了Pt-Ba-Ce /γ-Al<sub>2sub>O<sub>3subγ-Al<sub>2sub>O<sub>3sub> 上,X 射线光电子能谱(XPS)检测到Ce3+ 和Ce4+ 之间的差异,Ce3+ 和Ce4+ 促进了活性氧在催化剂上的迁移。在NO<sub>xsub> 吸附和脱附循环实验中,随着H<sub>2sub>暴露时间(30 s、45 s 和60 s)延长,NO<sub>xsub> 的存储效率和转化率增加适当增加H<sub>2sub>量加速了硝酸盐或亚硝酸盐的分解,有利于NO<sub>xsub> 存储-还原,并促进了下一循环NSR吸附位点的再生。

关键词: Pt–Ba–Ce/γ-Al<sub>2sub>O<sub>3sub> 催化剂,物理化学性质,NO<sub>xsub>存储和还原,NO<sub>xsub> 排放,H<sub>2sub> 还原剂    

Ultrasound-assisted co-precipitation synthesis of mesoporous Co3O4–CeO2 composite oxides for highly selective

《化学科学与工程前沿(英文)》 2022年 第16卷 第8期   页码 1211-1223 doi: 10.1007/s11705-022-2145-3

摘要: The one-step highly selective oxidation of cyclohexane into cyclohexanone and cyclohexanol as the essential intermediates of nylon-6 and nylon-66 is considerably challenging. Therefore, an efficient and low-cost catalyst must be urgently developed to improve the efficiency of this process. In this study, a Co3O4–CeO2 composite oxide catalyst was successfully prepared through ultrasound-assisted co-precipitation. This catalyst exhibited a higher selectivity to KA-oil, which was benefited from the synergistic effects between Co3+/Co2+ and Ce4+/Ce3+ redox pairs, than bulk CeO2 and/or Co3O4. Under the optimum reaction conditions, 89.6% selectivity to KA-oil with a cyclohexane conversion of 5.8% was achieved over Co3O4–CeO2. Its catalytic performance remained unchanged after five runs. Using the synergistic effects between the redox pairs of different transition metals, this study provides a feasible strategy to design high-performance catalysts for the selective oxidation of alkanes.

关键词: Co3O4–CeO2 composite oxides     cyclohexanone     cyclohexanol     ultrasonic-assisted co-precipitation     selective oxidation     solvent-free    

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    

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    

Optimization of the O/HO process with response surface methodology for pretreatment of mother liquor

《环境科学与工程前沿(英文)》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1371-5

摘要:

• Real ML-GFW with high salinity and high organics was degraded by O3/H2O2 process.

关键词: High salinity     High organic matters     Gas field wastewater     O3/H2O2     Response surface methodology    

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    

On the monolayer dispersion behavior of Co<sub>3sub>O<sub>4sub> on HZSM-5 support: designing applicable

《化学科学与工程前沿(英文)》 2023年 第17卷 第11期   页码 1741-1754 doi: 10.1007/s11705-023-2332-x

摘要: Based on monolayer dispersion theory, Co3O4/ZSM-5 catalysts with different loadings have been prepared for selective catalytic reduction of nitrogen oxides by ammonia. Co3O4 can spontaneously disperse on HZSM-5 support with a monolayer dispersion threshold of 0.061 mmol 100 m–2, equaling to a weight percentage around 4.5%. It has been revealed that the quantities of surface active oxygen (O2) and acid sites are crucial for the reaction, which can adsorb and activate NOx and NH3 reactants effectively. Below the monolayer dispersion threshold, Co3O4 is finely dispersed as sub-monolayers or monolayers and in an amorphous state, which is favorable to generate the two kinds of active sites, hence promoting the performance of ammonia selective catalytic reduction of nitrogen oxide. However, the formation of crystalline Co3O4 above the capacity is harmful to the reaction performance. 4% Co3O4/ZSM-5, the catalyst close to the monolayer dispersion capacity, possesses the most abundant active O2 species and acidic sites, thereby demonstrating the best reaction performance in all the samples. It is proposed the optimal Co3O4/ZSM-5 catalyst can be prepared by loading the capacity amount of Co3O4 onto HZSM-5 support.

关键词: Co3O4/ZSM-5     NOx-SCR by NH3     monolayer dispersion threshold effect     surface acid sites     surface active O2 anions    

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    

标题 作者 时间 类型 操作

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

范慧,宋世栋,韩敏芳

期刊论文

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

电解用Fe-Ni-Co-Al<sub>2sub>O<sub>3sub>金属陶瓷惰性阳极

邱竹贤,石忠宁,徐君莉

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

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

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

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

H<sub>2sub> 对Pt-Ba-Ce /γ-Al<sub>2sub>O<sub>3sub> 催化剂NO<sub>xsub> 存储和还原机理的影响研究

王攀, 裔静, 孙川, 罗鹏, 雷利利

期刊论文

Ultrasound-assisted co-precipitation synthesis of mesoporous Co3O4–CeO2 composite oxides for highly selective

期刊论文

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

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

Optimization of the O/HO process with response surface methodology for pretreatment of mother liquor

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

On the monolayer dispersion behavior of Co<sub>3sub>O<sub>4sub> on HZSM-5 support: designing applicable

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