燃料化学学报（中英文）2024，Vol.52Issue(1)：76-86,11.DOI:10.19906/j.cnki.JFCT.2023063
γ-Mo2N/C催化剂的合成及其甲酸脱氢性能研究
Synthesis of γ-Mo2N/C catalysts and its performance on formic acid dehydrogenation
路军 1王美君 2王志青 3董立波 3余钟亮 4常丽萍2
作者信息
- 1. 太原理工大学 省部共建煤基能源清洁高效利用国家重点实验室,山西太原 030024||太原理工大学 煤科学与技术教育部重点实验室,山西太原 030024||中国科学院山西煤炭化学研究所 煤炭转化国家重点实验室,山西太原 030024
- 2. 太原理工大学 省部共建煤基能源清洁高效利用国家重点实验室,山西太原 030024||太原理工大学 煤科学与技术教育部重点实验室,山西太原 030024
- 3. 中国科学院山西煤炭化学研究所 煤炭转化国家重点实验室,山西太原 030024
- 4. 上饶师范大学 化学与环境科学学院,江西上饶 334001
- 折叠
摘要
Abstract
Formic acid(FA)has received much attention due to its high hydrogen content(4.4％),easy H2 production and synthesis from small platform compounds.γ-Mo2N/C is very selective for the decomposition of FA along the H2 and CO2 pathways,generating very little CO and showing high application value.In this study,γ-Mo2N/C catalysts were prepared using aqueous p-phenylenediamine and ammonium molybdate solutions as precursors,and their FA decomposition performance was evaluated in-situ.The adsorption conformation of FA on the crystalline surface of γ-Mo2N(200)was calculated by DFT,and on this basis,the catalyst performance and the decomposition mechanism of FA on its surface were investigated.The results showed that γ-Mo2N/C exhibited very high catalytic activity at low temperatures and that improving the dispersion of γ-Mo2N on the C carrier was effective in improving the FA conversion.The best catalytic performance was achieved at a molar ratio of 4∶1 between p-phenylenediamine and ammonium molybdate,and the catalyst showed stable performance and high H2 selectivity(N2 40 mL/min,CO＜5.0×10-5)in the FA decomposition experiments at 160 ℃ and 100 h.DFT calculations showed that the H atom of the O-H bond in FA was more likely to bind to the N atom on the crystalline surface of γ-Mo2N/C(200),while the O atom of the C=O bond are more likely to bind to Mo atoms on the γ-Mo2N/C(200)crystal plane.The above results help to clarify the mechanism of FA decomposition under the action of γ-Mo2N/C and show the potential application of the non-precious metal catalyst γ-Mo2N/C in the decomposition of FA for H2 production.关键词
煤基衍生物利用/甲酸制氢/γ-Mo2N/负载型催化剂/氢能Key words
coal-based derivatives utilization/hydrogen production from formic acid/γ-Mo2N/loaded catalyst/hydrogen energy分类
化学化工引用本文复制引用
路军,王美君,王志青,董立波,余钟亮,常丽萍..γ-Mo2N/C催化剂的合成及其甲酸脱氢性能研究[J].燃料化学学报（中英文）,2024,52(1):76-86,11.
