共查询到20条相似文献，搜索用时 11 毫秒
1.
过量化石能源的消耗导致大气中的二氧化碳含量不断上升,由此引发包括温室效应在内的环境问题。对此,常温常压下的电催化二氧化碳还原手段为制备高附加值的化工原料和实现碳循环提供了一种很有前景的技术储备。在众多的二氧化碳还原产物中,碳氢化合物尤其是乙烯,它作为塑料和其他化工产品的重要原料受到广泛的关注。电催化二氧化碳还原制乙烯工艺不仅可适配于现有的生产设备也可作为取代目前工业化的裂解方法。近年来,研究者们为了开发高效的电催化二氧化碳还原制乙烯催化剂开展了大量的研究。不过值得注意的是,大部分研究集中于铜基材料。尽管目前研究者取得了很多成果,但仍缺少可高选择性产乙烯的二氧化碳还原催化剂。如何设计出可活化二氧化碳分子,同时对*CO和*COH中间物有强吸附能力的催化剂是研究难点。针对此问题,本文中通过真空蒸镀的方法制备出一种富氧空位的非晶氧化铜纳米薄膜催化剂。受益于纳米薄膜的构建和氧空位的引入,该催化剂可快速进行电荷和物质的交换,并利于二氧化碳分子的吸附及优化还原中间产物的亲和力,进而表现出优异的电催化二氧化碳制乙烯的性能。结果表明,在加有0.1 mol·L-1碳酸氢钾溶液的H型电... 相似文献
2.
采用改进的Hummers法制备了氧化石墨烯(GO),经水合肼还原得到石墨烯(RGO),通过浸渍法制备了石墨烯负载的镍基催化剂(Ni/RGO);对其催化二氧化碳甲烷化反应的性能进行了研究,并与以碳纳米管(CNTs)和活性炭(AC)为载体负载的Ni基催化剂进行了比较.由于催化剂的载体分别为RGO,CNTs和AC,所以Ni将会表现出不同的形态.利用红外光谱(FTIR)、比表面积(BET)测试、程序升温还原(H2-TPR)、X射线衍射(XRD)分析和透射电子显微镜(TEM)等表征手段对其结构及物理性质进行了表征.结果表明,Ni/RGO具有相对较大的比表面积(316 m~2/g),Ni在Ni/RGO上的颗粒尺寸(5.3 nm)小于其在Ni/CNTs(8.9 nm)和Ni/AC(11.6 nm)上的颗粒尺寸;该催化剂在二氧化碳甲烷化反应中具有更高的催化活性和选择性,而且具有良好的使用寿命. 相似文献
3.
Yucheng Cao Suya Chen Shuowen Bo Dr. Wenjun Fan Jiangnan Li Dr. Chunmei Jia Prof. Dr. Zhen Zhou Prof. Dr. Qinghua Liu Dr. Lirong Zheng Prof. Dr. Fuxiang Zhang 《Angewandte Chemie (International ed. in English)》2023,62(30):e202303048
Single atom alloy (SAA) catalysts have been recently explored for promotion of various heterogeneous catalysis, but it remains unexplored for selective electrocatalytic reduction of carbon dioxide (CO2) into multi-carbon (C2+) products involving C−C coupling. Herein we report a single-atomic Bi decorated Cu alloy (denoted as BiCu-SAA) electrocatalyst that could effectively modulate selectivity of CO2 reduction into C2+ products instead of previous C1 ones. The BiCu-SAA catalyst exhibits remarkably superior selectivity of C2+ products with optimal Faradaic efficiency (FE) of 73.4 % compared to the pure copper nanoparticle or Bi nanoparticles-decorated Cu nanocomposites, and its structure and performance can be well maintained at current density of 400 mA cm−2 under the flow cell system. Based on our in situ characterizations and density functional theory calculations, the BiCu-SAA is found to favor the activation of CO2 and subsequent C−C coupling during the electrocatalytic reaction, as should be responsible for its extraordinary C2+ selectivity. 相似文献
4.
Dr. Wenpeng Ni Prof. Yongji Guan Houjun Chen Prof. Yan Zhang Prof. Shuangyin Wang Prof. Shiguo Zhang 《Angewandte Chemie (International ed. in English)》2023,62(37):e202303233
Balancing the activation of H2O is crucial for highly selective CO2 electroreduction (CO2RR), as the protonation steps of CO2RR require fast H2O dissociation kinetics, while suppressing hydrogen evolution (HER) demands slow H2O reduction. We herein proposed one molecular engineering strategy to regulate the H2O activation using aprotic organic small molecules with high Gutmann donor number as a solvation shell regulator. These organic molecules occupy the first solvation shell of K+ and accumulate in the electrical double layer, decreasing the H2O density at the interface and the relative content of proton suppliers (free and coordinated H2O), suppressing the HER. The adsorbed H2O was stabilized via the second sphere effect and its dissociation was promoted by weakening the O−H bond, which accelerates the subsequent *CO2 protonation kinetics and reduces the energy barrier. In the model electrolyte containing 5 M dimethyl sulfoxide (DMSO) as an additive (KCl-DMSO-5), the highest CO selectivity over Ag foil increased to 99.2 %, with FECO higher than 90.0 % within −0.75 to −1.15 V (vs. RHE). This molecular engineering strategy for cation solvation shell can be extended to other metal electrodes, such as Zn and Sn, and organic molecules like N,N-dimethylformamide. 相似文献
5.
Yi-Feng Wang Li-Na Song Li-Jun Zheng Yue Wang Jia-Yi Wu Prof. Ji-Jing Xu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2024,136(17):e202400132
Li−CO2 batteries have received significant attention owing to their advantages of combining greenhouse gas utilization and energy storage. However, the high kinetic barrier between gaseous CO2 and the Li2CO3 product leads to a low operating voltage (<2.5 V) and poor energy efficiency. In addition, the reversibility of Li2CO3 has always been questioned owing to the introduction of more decomposition paths caused by its higher charging plateau. Here, a novel “trinity” Li−CO2 battery system was developed by synergizing CO2, soluble redox mediator (2,2,6,6-tetramethylpiperidoxyl, as TEM RM), and reduced graphene oxide electrode to enable selective conversion of CO2 to Li2C2O4. The designed Li−CO2 battery exhibited an output plateau reaching up to 2.97 V, higher than the equilibrium potential of 2.80 V for Li2CO3, and an ultrahigh round-trip efficiency of 97.1 %. The superior performance of Li−CO2 batteries is attributed to the TEM RM-mediated preferential growth mechanism of Li2C2O4, which enhances the reaction kinetics and rechargeability. Such a unique design enables batteries to cope with sudden CO2-deficient environments, which provides an avenue for the rationally design of CO2 conversion reactions and a feasible guide for next-generation Li−CO2 batteries. 相似文献
6.
7.
8.
9.
10.
石墨烯负载高活性Pd催化剂对乙醇的电催化氧化 总被引：4，自引：0，他引：4
以石墨粉为原料,采用Hummers法液相氧化合成了氧化石墨(GO),然后用化学一步还原制得石墨烯负载钯催化剂.X射线衍射(XRD)、透射电镜(TEM)表征表明,Pd在石墨烯载体上有较好的分散度,粒径为3-5nm.电化学活性面积(EASA)、循环伏安(CV)、计时电流(CA)和计时电位(CP)等电化学测试表明,与传统Pd/VulcanXC-72相比,Pd/石墨烯催化剂对碱性介质中乙醇电催化氧化的催化活性有了很大的提高. 相似文献
11.
12.
13.
14.
15.
16.
17.
18.
19.
20.