摘要
分别以CuCl2和维生素C为Cu源和绿色还原剂,MIL‑101(Cr)为多孔载体,采用双溶剂法直接将CuCl2引入MIL‑101(Cr)孔道内并全部还原成CuCl,成功实现了在金属有机骨架材料上构筑Cu活性位。结果表明,双溶剂法不会影响载体MIL‑101(Cr)的结构,引入的铜物种全部被选择性地还原成CuCl。当CuCl负载量为2.85 mmol·g^-1时,吸附剂对噻吩的吸附性能达到最佳,饱和吸附量为0.175 mmol·g^-1,明显高于载体MIL‑101(Cr)的0.112 mmol·g^-1。本策略实现了在温和条件下高效可控地制备Cu功能化吸附剂,其丰富的Cu位点和高孔隙率使得该吸附剂具有较好的吸附脱硫性能。
Herein,a representative metal‑organic framework(MOF),MIL‑101(Cr),with a large specific surface area and good hydrothermal stability,has been chosen as porous support.The introducing of Cuprecursor and reduction to Cuwere sequentially occurred in the pores of MIL‑101(Cr)via double‑solvent method(DSM)in which the CuCl2 was directly used for reduction and vitamin C was employed as a green reductant.The DSM is effective in preparing Cusites on support MIL‑101(Cr).By using the DSM,it can ensure that the structure of support material was maintained on account of mild operating conditions and all copper species in MIL‑101(Cr)were reduced to Cu.When CuCl content was 2.85 mmol·g^-1,the obtained Cu‑containing materials exhibited a thiophene adsorption capacity(up to 0.175 mmol·g^-1),obviously higher than that of pristine MIL‑101(Cr)(0.112 mmol·g^-1).This method thus offers a useful,controllable and green approach to form Cusites within MOFs under relatively facile conditions.The resultant adsorbents exhibit obviously enhanced adsorptive desulfurization performance because of the specific interaction between Cuand thiophenic sulfur compounds.
作者
李玉霞
李帅帅
刘晓勤
孙林兵
LI Yu‑Xia;LI Shuai‑Shuai;LIU Xiao‑Qin;SUN Lin‑Bing(State Key Laboratory of Materials-Oriented Chemical Engineering,College of Chemical Engineering,Nanjing Tech University,Nanjing 211816,China)
出处
《无机化学学报》
SCIE
CAS
CSCD
北大核心
2021年第2期259-266,共8页
Chinese Journal of Inorganic Chemistry
基金
国家自然科学基金(No.21722606、21676138和21878149)
中国博士后科学基金(No.51201370)资助。
关键词
脱硫
吸附
π作用
金属有机骨架
还原
desulfurization
adsorption
πinteractions
metal‑organic frameworks
reduction
