La-Stabilized, Single-Atom Ir/AC Catalyst for Heterogeneous Methanol Carbonylation to Methyl Acetate

被引:29
作者
Feng, Siquan [1 ,3 ]
Song, Xiangen [1 ]
Ren, Zhou [1 ,3 ]
Ding, Yunjie [1 ,2 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[2] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
基金
国家重点研发计划;
关键词
VAPOR-PHASE CARBONYLATION; ACETIC-ACID; ACTIVE-SITE; IRIDIUM; REACTIVITY; LIGANDS; POLYMER; ETHANOL; IODIDE;
D O I
10.1021/acs.iecr.8b05402
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Although homogeneous methanol carbonylation is industrialized to produce acetic acid, it still suffers from the problems of difficult separation and metal leaching. Here, we report a heterogeneous single atom Ir-La/AC catalyst to produce methyl acetate in a fixed-bed reactor. A high TOF of 2200h(-1) and high selectivity over 90% for methyl acetate with space time yield of 8200 g/(kg(cat) h) were achieved over the Ir-La/AC catalyst. Furthermore, the effects of reaction temperature, partial pressure of CO and CH3OH, weight ratio of CH3I/CH3OH, total LHSV as well as the role of La on the catalytic performance of Ir/AC were tested in this paper. In addition, we proposed a reasonable mechanism for heterogeneous methanol carbonylation over La stabilized single atom Ir/AC catalyst. Our work provides a reference for the further scale-up of the process and a stable, supported, single-atom system as a substitution for other homogeneous catalyst.
引用
收藏
页码:4755 / 4763
页数:9
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