C2H2与C2H2/CO2或C2H2/CO2/CH4混合物的有效分离对于实现高纯度C2H2(>99%)至关重要,这对于生产当代商品化学品至关重要。
该文中,研究人员介绍了一种金属-有机框架,ZNU-12,其具有由无机氟化阴离子形成的空间划分孔,用于高效的C2H2/CO2或C2H2/CO2/CH4分离。该框架由氟化SiF62–阴离子划分为三个不同的笼状物,能够同时实现高的C2H2容量(在298K和1.0bar下为176.5 cm3/g)和优异的C2H2对CO2(13.4)和CH4(233.5)的选择性。
值得注意的是,通过高回收率的吸附-解吸突破实验循环,我们从C2H2/CO2(v/v=50/50)和C2H2/CO2/CH4(v/v=1/1/1、1/1/2或1/1/8)混合物中获得了创纪录的C2H2生产率(132.7、105.9、98.8和80.0 L/kg,纯度99.5%)。理论计算表明,在受限空腔中,C2H2和两个六氟硅酸盐(SiF62-)阴离子之间存在有效的“2+2”协同氢键。
附:英文原文
Title: Metal–Organic Framework with Space-Partition Pores by Fluorinated Anions for Benchmark C2H2/CO2 Separation
Author: Yuanbin Zhang, Yan Han, Binquan Luan, Lingyao Wang, Wenlei Yang, Yunjia Jiang, Teng Ben, Yabing He, Banglin Chen
Issue&Volume: June 11, 2024
Abstract: The efficient separation of C2H2 from C2H2/CO2 or C2H2/CO2/CH4 mixtures is crucial for achieving high-purity C2H2 (>99%), essential in producing contemporary commodity chemicals. In this report, we present ZNU-12, a metal–organic framework with space-partitioned pores formed by inorganic fluorinated anions, for highly efficient C2H2/CO2 and C2H2/CO2/CH4 separation. The framework, partitioned by fluorinated SiF62– anions into three distinct cages, enables both a high C2H2 capacity (176.5 cm3/g at 298 K and 1.0 bar) and outstanding C2H2 selectivity over CO2 (13.4) and CH4 (233.5) simultaneously. Notably, we achieve a record-high C2H2 productivity (132.7, 105.9, 98.8, and 80.0 L/kg with 99.5% purity) from C2H2/CO2 (v/v = 50/50) and C2H2/CO2/CH4 (v/v = 1/1/1, 1/1/2, or 1/1/8) mixtures through a cycle of adsorption–desorption breakthrough experiments with high recovery rates. Theoretical calculations suggest the presence of potent “2 + 2” collaborative hydrogen bonds between C2H2 and two hexafluorosilicate (SiF62–) anions in the confined cavities.
DOI: 10.1021/jacs.4c03442
Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c03442
JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:16.383
官方网址:https://pubs.acs.org/journal/jacsat
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