The importance of constructing Triple-functional Sr2P2O7/Ni2P catalysts for smoothing hydrogenation Ring-rearrangement of Biomass-derived Furfural compounds in water

化学 催化作用 异构化 环戊酮 糠醛 密度泛函理论 动力学同位素效应 药物化学 立体化学 计算化学 有机化学 量子力学 物理
作者
Chao Cheng,Cheng-shan Zhao,Dan Zhao,Shunmin Ding,Chao Chen
出处
期刊:Journal of Catalysis [Elsevier BV]
卷期号:421: 117-133 被引量:19
标识
DOI:10.1016/j.jcat.2023.03.007
摘要

Rational design of catalysts with multi-function was of great importance for speeding mechanism-complicated heterogeneous reaction. Herein, a series of Sr-Ni-P catalysts characterized in (Sr2P2O7)m/Ni2P composite structure (Sr:Ni molar ratio m = 0.15–0.60) were prepared and investigated for hydrogenation ring-rearrangement of four biomass-derived Furfural compounds (FALs) to their Cyclopentanone derivatives (CPOs) in water. By properly manipulate m at 0.40, the superior and reproducible CPOs yields up to 96% were achieved under mild conditions in particular under low-pressure (0.1 MPa) H2. Chemical adsorption measurements disclosed that the attachment of Sr2P2O7 with Ni2P in nanoscale was crucial to construct triple-functional catalytic interface with modulated hydrogen activation (7.5–47.4 µmol/g), acid (196.4–327.3 µmol/g) and base (108.0–214.5 µmol/g) sites. H2-D2 exchange, H2-IR experiments and DFT simulation implied that H2 could be activated through heterolytic dissociation on Sr2P2O7 to participate in reaction; H218O, D2O, D2 isotope-label tracing experiments and DFT mechanism calculation further clarified that besides of H2, H2O was also frequently present in hydrogenation, ring opening, rearrangement and ring re-closing steps and acted as dual donors to provide H and O for CPO; in the favorable thermodynamic feature, a new pathway (with unsaturated dicarbonyl compound as key intermediate) achieved on Sr2P2O7/Ni2P was demonstrated to be more feasible than the reported pathway. The importance of the triple-functional Sr2P2O7/Ni2P catalytic interface for smoothing the aqueous hydrogenation transformation, in particular the function of base site for speeding the transformation was illustrated and discussed.
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
刚刚
万能图书馆应助郭小胖14采纳,获得10
1秒前
2秒前
black发布了新的文献求助10
2秒前
梦XING发布了新的文献求助10
2秒前
思睿观通发布了新的文献求助10
2秒前
2秒前
2秒前
3秒前
3秒前
CXQCXQ发布了新的文献求助10
4秒前
大傻春发布了新的文献求助10
5秒前
5秒前
今后应助高lucky采纳,获得10
5秒前
5秒前
啊懂发布了新的文献求助10
5秒前
酷波er应助Rockyhee22采纳,获得10
6秒前
姚姚的赵赵完成签到,获得积分10
6秒前
6秒前
研友_LBKR9n发布了新的文献求助10
7秒前
鱼鱼鱼完成签到,获得积分10
7秒前
ziyu发布了新的文献求助10
7秒前
家伟发布了新的文献求助10
7秒前
JamesPei应助愤怒的含雁采纳,获得10
7秒前
yuiiuy发布了新的文献求助150
7秒前
李健的小迷弟应助77采纳,获得10
7秒前
曹博发布了新的文献求助10
7秒前
ncjdoi发布了新的文献求助10
8秒前
我的文献呢应助Sunwenrui采纳,获得30
8秒前
8秒前
PAD发布了新的文献求助30
8秒前
9秒前
深情安青应助jerkran采纳,获得50
9秒前
风清扬发布了新的文献求助10
9秒前
Akim应助kgrvlm采纳,获得10
9秒前
wjx发布了新的文献求助10
9秒前
10秒前
wangbin743完成签到,获得积分10
10秒前
吭吭唧唧完成签到,获得积分10
10秒前
11秒前
高分求助中
Picture Books with Same-sex Parented Families: Unintentional Censorship 700
ACSM’s Guidelines for Exercise Testing and Prescription, 12th edition 500
Nucleophilic substitution in azasydnone-modified dinitroanisoles 500
不知道标题是什么 500
Indomethacinのヒトにおける経皮吸収 400
Phylogenetic study of the order Polydesmida (Myriapoda: Diplopoda) 370
Effective Learning and Mental Wellbeing 300
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 3974844
求助须知:如何正确求助?哪些是违规求助? 3519270
关于积分的说明 11197844
捐赠科研通 3255496
什么是DOI,文献DOI怎么找? 1797791
邀请新用户注册赠送积分活动 877187
科研通“疑难数据库(出版商)”最低求助积分说明 806202