Chemical Engineering Science ( IF 4.7 ) Pub Date : 2022-06-23 , DOI: 10.1016/j.ces.2022.117827 Jinxing Mi , Guanqing Zhang , Qiuyun Zhang , Weitao Zhao , Yanning Cao , Fujian Liu , Lilong Jiang
Adsorption and dissociation of H2O along with the generated hydroxide ions (OH–) over catalyst plays key role in the carbonyl sulfur (COS) hydrolysis. Herein, we report a variety of magnesium aluminum layered double hydroxides nanosheet with abundant structural defects (MA-LDHs-SD-x) designed by a mechanochemistry method using white carbon black as the defects directing agent. The resulted MA-LDHs-SD-x possess abundant structural defects along with much enlarged BET surface area and pore volume (175 m2/g and 0.347 cm3/g vs 32 m2/g and 0.039 cm3/g), which provide enhanced amount of surface OH– base sites, tight and rigid diffusion channels for guest molecules. As expected, the MA-LDHs-SD-x were found to be rather active in catalyzing COS hydrolysis, nearly 100% conversion and selectivity can be achieved at only 30 °C without H2O in a span of 96 h through a hydroxyl chemical looping route, which showing potential application value in the industrial desulfuration.
中文翻译:
MgAl-水滑石纳米片上的缺陷调控,通过羟基化学循环途径改善羰基硫消除性能
H 2 O 与生成的氢氧根离子 (OH – ) 在催化剂上的吸附和解离在羰基硫 (COS) 水解中起关键作用。在此,我们报道了多种结构缺陷丰富的镁铝层状双氢氧化物纳米片(MA-LDHs-SD-x),采用机械化学方法,使用白炭黑作为缺陷导向剂。得到的 MA-LDHs-SD-x 具有丰富的结构缺陷,同时 BET 表面积和孔体积也大大增加(175 m 2 /g 和 0.347 cm 3 /g vs 32 m 2 /g 和 0.039 cm 3 /g),这提供更多的表面 OH –客体分子的碱基位点,紧密而刚性的扩散通道。正如预期的那样,发现 MA-LDHs-SD-x 在催化 COS 水解方面具有相当的活性,在没有 H 2 O 的情况下,仅在 30 °C 下通过羟基化学品在 96 小时内即可实现近 100% 的转化率和选择性。循环路线,在工业脱硫中显示出潜在的应用价值。