Mechanism insights into direct conversion of syngas into C2 oxygenates via key intermediate C2O2 over Ni-Supported graphene

石墨烯 合成气 催化作用 氧合物 化学 乙二醇 乙二醛 材料科学 光化学 纳米技术 有机化学
作者
Pengfei Liu,Yanhui Yang,Qiang Wang
出处
期刊:Carbon [Elsevier BV]
卷期号:175: 322-333 被引量:3
标识
DOI:10.1016/j.carbon.2021.01.008
摘要

A critical step toward the rational design of new catalyst that achieve selective and efficient synthesis of C2+ oxygenates from syngas (CO/H2) by Fischer-Tropsch synthesis (FTS) is to determine the detailed reaction mechanism. Herein, the mechanism of two gaseous CO monomers coupling into a chemisorbed ethylene dione (O∗C∗CO) and subsequent hydrogenation of O∗C∗CO on the chainmail catalyst of nickel-supported graphene surface is reported. The results show that two gaseous CO monomers can be coupled into a two-atom-chemisorbed O∗C∗CO via a metastable intermediate of O∗CCO single-atom-chemisorbed on Ni-supported on graphene with the barrier energy of 0.85 eV and a strong exothermicity of 1.45 eV. The key intermediate of O∗C∗CO can be stably chemisorbed on the Ni-supported-graphene surface by riveting two coupled C atoms on the ortho-, meta-, or para-position of graphene six-membered ring, forming four-, five-, and six-membered ring with the carbon atoms of graphene, respectively. Then, the potential energy surfaces of chemisorbed O∗C∗CO hydrogenation indicates that glycol-aldehyde (HOH2C–CHO) would be preferred to form by the kinetically favorable initial C-hydrogenation due to the low rate-limiting barrier of 0.46 eV, while the glyoxal (OHC=CHO) is a considerably competitive product because its rate-limiting barrier is only 0.18 eV higher than that of the glycol-aldehyde. These results suggest that the chainmail catalyst of nickel-supported graphene could be a potential and high-efficient catalyst for synthesis of C2 oxygenates from syngas, which also provides a fundamental insight into the new reaction mechanism of Fischer-Tropsch synthesis.
最长约 10秒,即可获得该文献文件

科研通智能强力驱动
Strongly Powered by AbleSci AI
更新
PDF的下载单位、IP信息已删除 (2025-6-4)

科研通是完全免费的文献互助平台,具备全网最快的应助速度,最高的求助完成率。 对每一个文献求助,科研通都将尽心尽力,给求助人一个满意的交代。
实时播报
科研达人发布了新的文献求助30
2秒前
RogerCqz完成签到 ,获得积分10
3秒前
4秒前
jiang发布了新的文献求助10
4秒前
圆锥香蕉应助科研通管家采纳,获得20
5秒前
怕黑半仙应助科研通管家采纳,获得10
5秒前
5秒前
圆锥香蕉应助科研通管家采纳,获得20
5秒前
科研通AI5应助科研通管家采纳,获得10
5秒前
5秒前
领导范儿应助科研通管家采纳,获得10
5秒前
6秒前
6秒前
Cml完成签到,获得积分10
7秒前
Liufgui应助牛文文采纳,获得10
8秒前
chun发布了新的文献求助10
9秒前
YI应助南兮采纳,获得10
9秒前
orixero应助颜云尔采纳,获得10
10秒前
anna发布了新的文献求助10
10秒前
YWang发布了新的文献求助10
13秒前
13秒前
NiNi完成签到,获得积分10
15秒前
悦耳寒松发布了新的文献求助10
15秒前
sijing发布了新的文献求助10
16秒前
7777完成签到,获得积分10
16秒前
求求了,让孩子毕业吧完成签到,获得积分10
17秒前
17秒前
20秒前
我是老大应助LiuJinhui采纳,获得10
21秒前
24秒前
量子星尘发布了新的文献求助10
24秒前
清久完成签到,获得积分10
25秒前
牛马码字员完成签到,获得积分10
25秒前
橙果果发布了新的文献求助20
26秒前
所所应助11采纳,获得10
26秒前
tt大耳朵完成签到,获得积分10
27秒前
27秒前
28秒前
枫之林发布了新的文献求助10
28秒前
辛俊辰发布了新的文献求助10
28秒前
高分求助中
A new approach to the extrapolation of accelerated life test data 1000
ACSM’s Guidelines for Exercise Testing and Prescription, 12th edition 500
‘Unruly’ Children: Historical Fieldnotes and Learning Morality in a Taiwan Village (New Departures in Anthropology) 400
Indomethacinのヒトにおける経皮吸収 400
Phylogenetic study of the order Polydesmida (Myriapoda: Diplopoda) 370
基于可调谐半导体激光吸收光谱技术泄漏气体检测系统的研究 350
Robot-supported joining of reinforcement textiles with one-sided sewing heads 320
热门求助领域 (近24小时)
化学 材料科学 医学 生物 工程类 有机化学 生物化学 物理 内科学 纳米技术 计算机科学 化学工程 复合材料 遗传学 基因 物理化学 催化作用 冶金 细胞生物学 免疫学
热门帖子
关注 科研通微信公众号,转发送积分 3989069
求助须知:如何正确求助?哪些是违规求助? 3531351
关于积分的说明 11253589
捐赠科研通 3269939
什么是DOI,文献DOI怎么找? 1804851
邀请新用户注册赠送积分活动 882074
科研通“疑难数据库(出版商)”最低求助积分说明 809073