Controlled Construction of Supported Cu+ Sites and Their Stabilization in MIL-100(Fe): Efficient Adsorbents for Benzothiophene Capture
Controlled Construction of Supported Cu+ Sites and Their Stabilization in MIL-100(Fe): Efficient Adsorbents for Benzothiophene Capture
复制标题
MIL-100(Fe) 中负载铜位点的受控构建及其稳定性：苯并噻吩捕获的高效吸附剂
DOI：
10.1021/acsami.7b09300
复制
发表时间：
2017
影响因子：
9.5
通讯作者：
Sun Lin-Bing
中科院分区：
文献类型：
--
作者：
He Qiu-Xia;Jiang Yao;Tan Peng;Liu Xiao-Qin;Qin Ju-Xiang;Sun Lin-Bing
含Cu+的材料由于其用途广泛、无毒、成本低廉而在各种应用中引起了广泛的关注。然而，选择性还原的困难和Cu+物种的稳定性差，现在几乎是议程。在此，通过蒸气还原策略（VRS）在温和条件（200 °C，5 h）下实现了MIL-100（Fe）中负载Cu+位点的受控构建。值得注意的是，Cu+的产率达到100%，这比传统的高温自还原方法高得多，即使在700 °C下12 h，产率也不到50%。更重要的是，在通过VRS处理期间，MIL-100（Fe）中的一些Fe 3+被还原为Fe 2+，这防止了由于Fe 2+的较高氧化电位而经常发生的Cu+的氧化。这些性质使得Cu+/MIL-100（Fe）在吸附容量和稳定性方面有效地捕获典型的芳香族硫，苯并噻吩。据我们所知，首次实现了利用载体的氧化倾向稳定Cu+，这可能为利用弱稳定性活性中心提供了新的思路。
Cu+-containing materials have drawn much attention in various applications because they are versatile, nontoxic, and low-cost. However, the difficulty of selective reduction and the poor stability of Cu+species are now pretty much the agendas. Here, controlled construction of supported Cu+sites in MIL-100(Fe) was realized under mild conditions (200 °C, 5 h) via a vapor-reduction strategy (VRS). Remarkably, the yield of Cu+reaches 100%, which is quite higher than the traditional high-temperature autoreduction method with a yield less than 50% even at 700 °C for 12 h. More importantly, during the treatment via VRS some Fe3+in MIL-100(Fe) are reduced to Fe2+, which prevent the frequently happened oxidation of Cu+due to the higher oxidation potential of Fe2+. These properties make Cu+/MIL-100(Fe) efficient in the capture of typical aromatic sulfur, benzothiophene, with regard to both adsorption capacity and stability. To our knowledge, the stabilization of Cu+using the oxidation tendency of supports is achieved for the first time, which may offer a new idea to utilize active sites with weak stability.