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121.
Gar B. Hoflund Steven D. Gardner David R. Schryer Billy T. Upchurch Erik J. Kielin 《Reaction Kinetics and Catalysis Letters》1996,58(1):19-26
The influence of promoters on Pt/SnOx/SiO2 and Au/MnOx low-temperature CO oxidation catalysts has been investigated under stoichiometric reaction conditions with no CO2 added to the feed gas. The performance of Pt/SnOx/SiO2 catalysts is improved significantly by the addition of 1 wt.% Fe but reduced by the addition of 5 wt.%Fe, 1 wt.% Sb, 5 wt.% Sb, 1 wt.% As, 5 wt.%As and 1.8 wt.% P. The performance of Au/MnOx is improved significantly by the addition of 1 at.% Ce but reduced by the addition of 1 at.% Co. For the catalysts and conditions examined, the Au/MnOx catalysts are superior to the Pt/SnOx/SiO2 catalysts with respect to both activity and decay characteristics. 相似文献
122.
报道了用脉冲反应研究Ni/Al2O3催化剂上CH4/CO2重整反应的结果。脉冲反应显示,在还原的Ni/Al2O3催化剂上,CH4在673K就开始发生分解,并有C2H6、C2H4生成,1023K下,CH4几乎完全分解,单纯的CO2则很难在还原的催化剂上发生反应,在973K以上的高温下才会有少量C胜成CO.CHCO2的脉冲反应表明,当CH4在较低温度下开始分解时,CO2也会发生分解,并生成CO。脉冲反 相似文献
123.
Fossil fuels are expected to be the major source of energy for the next few decades. However, combustion of nonrenewable resources leads to the release of large quantities of CO2, the primary greenhouse gas. Notably, the concentration of CO2 in the atmosphere is increasing annually at an astounding rate. Electrochemical CO2 reduction (ECR) to value-added fuels and chemicals using electricity from intermittent renewable energy sources is a carbon-neutral method to alleviate anthropogenic CO2 emissions. Despite the steady progress in the selective generation of C1 products (CO and formic acid), the production of multi-carbon species still suffers from low selectivity and efficiency. As an ECR product, ethylene (C2H4) has a higher energy density than do C1 species and is an important industrial feedstock in high demand. However, the conversion of CO2 to C2H4 is plagued by low productivity and large overpotential, in addition to the severe competing hydrogen evolution reaction (HER) during the ECR. To address these issues, the design and development of advanced electrocatalysts are critical. Here, we demonstrate fine-tuning of ECR to C2H4 by taking advantage of the prominent interaction of Cu with shape-controlled CeO2 nanocrystals, that is, cubes, rods, and octahedra predominantly covered with (100), (110), and (111) surfaces, respectively. We found that the selectivity and activity of the ECR depended strongly on the exposed crystal facets of CeO2. The overall ECR Faradaic efficiency (FE) over Cu/CeO2(110) (FE ≈ 56.7%) surpassed that of both Cu/CeO2(100) (FE ≈ 51.5%) and Cu/CeO2(111) (FE ≈ 48.4%) in 0.1 mol·L-1 KHCO3 solutions with an H-type cell. This was in stark contrast to the exclusive occurrence of the HER over pure carbon paper, CeO2(100), CeO2(110), and CeO2(111). In particular, the FE toward C2H4 formation and the partial current density increased in the sequence Cu/CeO2(111) < Cu/CeO2(100) < Cu/CeO2(110) within applied bias potentials from -1.00 to -1.15 V (vs. the reversible hydrogen electrode), reaching 39.1% over Cu/CeO2(110) at a mild overpotential (1.13 V). The corresponding values for Cu/CeO2(100) and Cu/CeO2(111) were FEC2H4 ≈ 31.8% and FEC2H4 ≈ 29.6%, respectively. The C2H4 selectivity was comparable to that of many reported Cu-based electrocatalysts at similar overpotentials. Furthermore, the FE for C2H4 remained stable even after 6 h of continuous electrolysis. The superior ECR activity of Cu/CeO2(110) to yield C2H4 was attributed to the metastable (110) surface, which not only promoted the effective adsorption of CO2 but also remarkably stabilized Cu+, thereby boosting the ECR to produce C2H4. This work offers an alternative strategy to enhance the ECR efficiency by crystal facet engineering. 相似文献
124.
Organic reactions in supercritical carbon dioxide (scCO2) have facilitated great progress in recent years . ScCO2, as an environmentally friendly reaction medium, may be a substitute for 1 volatile and toxic organic solvents and show some special advantages. Firstly, CO2 is inexpensive, nonflammable, nontoxic and chemical inert under many conditions. Secondly, scCO2 possesses hybrid properties of both liquid and gas, to the advantage of some reactions involving gaseous reagents. Control o… 相似文献
125.
中国无烟煤焦气化活性的研究——水蒸气与二氧化碳气化活性的比较 总被引:2,自引:7,他引:2
在常压和920℃~1050℃下,采用热重方法,进行了六种中国典型无烟煤焦水蒸气与二氧化碳气化活性比较的研究。结果表明,无烟煤焦与水蒸气气化反应的活性与无烟煤的煤化程度相对应,无烟煤煤化程度越高,水蒸气气化反应活性越小。无烟煤焦与二氧化碳气化反应的活性与煤中矿物质的催化作用有密切关系,煤中矿物质的催化作用越大,二氧化碳气化反应活性越大。无烟煤焦与二氧化碳气化反应活性明显小于与水蒸气气化反应活性,后者比前者大10倍左右。初步探讨了无烟煤焦与水蒸气和二氧化碳的气化机理。 相似文献
126.
采用非晶态多核配合的方法合成了La1-xCuxMnO3(x=0、0.05、0.1、0.2、0.3、0.4、0.5)系列催化剂, 并用X射线衍射(XRD)、透射电镜(TEM)、比表面测定仪(BET)等手段对催化剂的微观结构进行了表征. 研究了Cu掺杂对钙钛矿结构及其对CO催化氧化发光性能及催化氧化CO、CH4性能的影响规律. 结果表明, 当x≤0.1 时, Cu掺杂仍可形成单相的钙钛矿结构; 当x>0.1时, 过量掺杂的Cu以CuO杂相存在. Cu掺杂可改善La1-xCuxMnO3催化剂对CO和CH4的催化氧化活性. 经700 ℃焙烧3 h制备的La0.9Cu0.1MnO3催化剂具有最高CO催化氧化活性(T100%=170 ℃), 该结果与CO催化氧化发光结果一致.而La0.95Cu0.05MnO3催化剂对CH4的催化氧化活性最高(T95%=705 ℃). 相似文献
127.
PEMFC催化剂的研究:自制抗CO中毒Pt-Ru/C电催化剂的性质 总被引:4,自引:0,他引:4
用胶体法制备了抗CO中毒PEMFC阳极Pt-Ru/C电催化剂(标记为THYT-2),对 比研究了THYT-2与Johnson Matthey (JM)公司同类品牌Pt-Ru/C催化剂的电化学及 其它物理化学性能。结果表明,THYT-2电催化剂在甲醇燃料电池和CO/H_2(Φ_ (CO) = 1 * 10~(-4))的氢氧燃料电池中的电催化行为与JM催化剂相当,但THYT- 2在低浓度CO氢气燃料中的电池性能更好。两种催化剂的其它物理化学性质具有类 似性:XPS分析结果表明THYT-2和JM催化剂 中都有三种不同价态的Pt存在:即金 属态Pt(0)、氧化态Pt(II)和Pt(IV)。HRTEM测试结果表明两种催化剂的粒径处在2 ~3 mn左右,这可能是它们拥有良好电化学性能的主要原因之一。本文还对催化剂 中Pt与Ru组分的分布和相互作用进行了讨论,提出了改进Pt-Ru/C电催化剂的思路 。 相似文献
128.
129.
The cerium‐containing MCM‐41 (Ce‐MCM‐41) has been synthesized by direct hydrothermal method. The low‐angle XRD patterns revealed the typical five major peaks of MCM‐41 type hexagonal structures. The interplanar spacing d100 = 38.4 Å was obtained that can be indexed on a hexagonal unit cell parameter with ao = 44.3 Å which was larger than that of pure siliceous MCM‐41 (Si‐MCM‐41). Transmission electron micrograph shows the regular hexagonal array of uniform channel characteristics of MCM‐41. The BET surface area of Ce‐MCM‐41 was 840 m2/g, which is much reduced as compared to that of Si‐MCM‐41, with the pore size of 26.9 Å and mesopore volume of 0.78 cm3/g were measured by nitrogen adsorption‐desorption isotherm at 77 K. Along with the results, the synthesized Ce‐MCM‐41 exhibited a well‐ordered MCM‐41‐type mesoporous structure with the incorporation of cerium. Using Ce‐MCM‐41 as a support, the Rh (0.5 wt%) catalyst exhibited very high activity for the NO/CO reactions. 相似文献
130.
固体氧化物电解池是一种高效、环境友好型的能量转换器件,可以直接将电能转化为化学能. 本文介绍了近年来作者课题组在固体氧化物电解池直接用于CO2还原的研究进展,并以阴极材料为主着重讨论了金属陶瓷电极和混合导电型钙钛矿氧化物电极的研究工作,最后展望了未来固体氧化物电解池直接电解CO2的研究思路和方向. 相似文献