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具有调制d带中心的钯和锡在MXene上的工程支持和分布
作者:小柯机器人 发布时间:2022/9/21 14:20:54

中山大学曾志平团队提出了用于CO可恢复甲醇氧化的具有调制d带中心钯和锡在MXene上的工程支持和分布。相关研究成果于2022年9月16日发表于国际一流学术期刊《德国应用化学》。

直接甲醇燃料电池(DMFC)的效率在很大程度上取决于甲醇氧化反应(MOR)催化剂的活性和耐久性。

该文中,研究人员提出了一种通过渐进式一步电化学沉积策略,锚定在掺硒MXene(PdSn0.5/SeTi3C2)上的钯锡纳米合金CO可恢复MOR催化剂。Pd/Se Ti3C2催化剂(1046.2 mA mg-1)产生的MOR质量活性比Pd/Ti3C2大2倍以上,表明在MXene上引入硒原子可能会加速反应动力学。PdSn0.5/SeTi3C2与MXene的Se掺杂进程和Pd-Sn协同位点具有优越的MOR质量活性(4762.8 mA mg-1),优于许多其他报道的Pd基催化剂。

实验结果和理论计算均表明,金属晶体与掺硒MXene的增强电子相互作用和Pd-Sn位的优化分布可以调制d带中心,降低Pd位CO*的吸附能,并增强Sn位OH*的生成,通过与邻近锡位上的邻近OH物种反应,高效去除CO中间产物。

附:英文原文

Title: Engineering Support and Distribution of Palladium and Tin on MXene with the Modulation d-Band Center for CO-resilient Methanol Oxidation

Author: Shufen Chen, Ning Liu, Junjie Zhong, Rongliang Yang, Bo Yan, Liyong Gan, Peng Yu, Xuchun Gui, Hongbin Yang, Dingshan Yu, Zhiping Zeng, Guowei Yang

Issue&Volume: 2022-09-16

Abstract: The efficiency of direct methanol fuel cell (DMFC) is largely determined by the activity and durability of methanol oxidation reaction (MOR) catalysts. Herein, we present a CO-resilient MOR catalyst of palladium-tin nano-alloy anchored on Se-doped MXene (PdSn  0.5  /Se-Ti  3  C  2  ) via a progressive one-step electrochemical deposition strategy. MOR mass activity resulting from Pd/Se-Ti  3  C  2  catalyst (1046.2 mA mg  -1  ) is over 2-fold larger than that of Pd/Ti  3  C  2  , suggesting that the introduction of Se atoms on MXene might accelerate the reaction kinetics. PdSn  0.5  /Se-Ti  3  C  2  with Se-doping progress of MXene and the cooperated Pd-Sn sites has a superior MOR mass activity (4762.8 mA mg  -1  ), outperforming many other reported Pd-based catalysts. Both experimental results and theoretical calculation reveal that boosted electron interaction of metal crystals with Se-doped MXene and optimized distribution of Pd-Sn sites can modulate the d band center, reduce adsorption energies of CO* at Pd site and enhance OH* generation at Sn site, resulting in highly efficient removal of CO intermediates by reaction with neighboring OH species on adjacent Sn sites.

DOI: 10.1002/anie.202209693

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202209693

期刊信息

Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:12.959
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx