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用于CO吸附的MgCaAl层状双氢氧化物衍生的混合金属氧化物多孔六方纳米片

MgCaAl layered double hydroxide-derived mixed metal oxide porous hexagonal nanoplatelets for CO sorption.

作者信息

Nethravathi C, Rajamathi Michael

机构信息

Materials Research Group, St Joseph's University, 36, Lalbagh Road, Bangalore, 560027, India.

Department of Chemistry, Mount Carmel College, Bangalore 560052, India.

出版信息

Dalton Trans. 2024 Aug 20;53(33):14108-14116. doi: 10.1039/d4dt01647e.

DOI:10.1039/d4dt01647e
PMID:39120604
Abstract

Porous hexagonal nanoplatelets of mixed metal oxide (MMO) derived from the calcination of MgAl layered double hydroxide exhibits a CO sorption capacity of 1.99 mmol g at 30 °C, with a retention of 87% sorption capacity over 10 carbonation-decarbonation cycles and a CO sorption capacity of 1 mmol g at 200 °C with a 40% increase in capacity over 10 cycles. The high sorption capacity is attributed to the porous nanoplatelet structure of the MMO with a BET surface area of 115 m g, which enables increased CO diffusion. Upon partially replacing magnesium with calcium (33, 50 and 66 mol%), the CO sorption capacity of the MMO increases with an increase in temperature. MMO derived from LDH, in which 66% of magnesium is replaced by calcium (MgCaAl-66), delivers CO sorption capacities of 1.38, 1.31, 2.50, 4.85 and 7.75 mmol g at 200, 300, 350, 400 and 600 °C, respectively, which is significant for application in the sorption-enhanced water gas shift (SEWGS) process. MgCaAl-66 MMO exhibits a sorption capacity of 1 mmol g, which is stable over 10 cycles at 200 °C, and a sorption capacity of 3.68 mmol g at 400 °C with 85% capture efficiency retention over 10 cycles. While the incorporation of Ca serves multiple purposes such as increasing basic defect sorption sites and improving stability to repress the sintering-induced limitation of MMO over sorption cycles, the porous nanoplatelets act as individual sorbent units resisting volume changes through carbonation-decarbonation cycles.

摘要

由MgAl层状双氢氧化物煅烧得到的混合金属氧化物(MMO)多孔六边形纳米片在30°C时表现出1.99 mmol/g的CO吸附容量,在10次碳酸化-脱碳循环中吸附容量保留率为87%,在200°C时CO吸附容量为1 mmol/g,在10次循环中容量增加40%。高吸附容量归因于MMO的多孔纳米片结构,其BET表面积为115 m²/g,这使得CO扩散增加。用钙部分替代镁(33%、50%和66%摩尔比)后,MMO的CO吸附容量随温度升高而增加。由LDH衍生的MMO,其中66%的镁被钙替代(MgCaAl-66),在200、300、350、400和600°C时分别具有1.38、1.31、2.50、4.85和7.75 mmol/g的CO吸附容量,这对于吸附增强水煤气变换(SEWGS)过程的应用具有重要意义。MgCaAl-66 MMO在200°C时表现出1 mmol/g的吸附容量,在10次循环中保持稳定,在400°C时吸附容量为3.68 mmol/g,在10次循环中捕获效率保留率为85%。虽然掺入钙有多种作用,如增加碱性缺陷吸附位点和提高稳定性以抑制MMO在吸附循环中的烧结诱导限制,但多孔纳米片作为单个吸附剂单元,可抵抗碳酸化-脱碳循环中的体积变化。

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