Hydrogen generation from methanol at near-room temperature

被引:82
作者
Shen, Yangbin [1 ,2 ]
Zhan, Yulu [1 ]
Li, Shuping [1 ]
Ning, Fandi [1 ]
Du, Ying [1 ]
Huang, Yunjie [3 ]
He, Ting [1 ]
Zhou, Xiaochun [1 ,4 ]
机构
[1] Chinese Acad Sci, Suzhou Inst Nanotech & Nanobion, Div Adv Nanomat, Suzhou 215125, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] China Univ Geosci, Fac Mat Sci & Chem, Wuhan 430074, Hubei, Peoples R China
[4] Chinese Acad Sci, Suzhou Inst Nanotech & Nanobion, Key Lab Nanodevices & Applicat, Suzhou 215125, Peoples R China
基金
中国国家自然科学基金;
关键词
HETEROCYCLIC CARBENE COMPLEXES; FORMIC-ACID; IRIDIUM COMPLEX; MECHANISTIC INSIGHTS; ENZYMATIC REDUCTION; RUTHENIUM COMPLEX; CATALYTIC-SYSTEM; PINCER CATALYST; MILD CONDITIONS; FUEL-CELL;
D O I
10.1039/c7sc01778b
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
As a promising hydrogen storage medium methanol has many advantages such as a high hydrogen content (12.5 wt%) and low-cost. However, conventional methanol-water reforming methods usually require a high temperature (>200 degrees C). In this research, we successfully designed an effective strategy to fully convert methanol to hydrogen for at least 1900 min (similar to 32 h) at near-room temperature. The strategy involves two main procedures, which are CH3OH -> HCOOH -> H-2 and CH3OH -> NADH -> H-2. HCOOH and the reduced form of nicotinamide adenine dinucleotide (NADH) are simultaneously produced through the dehydrogenation of methanol by the cooperation of alcohol dehydrogenase (ADH) and aldehyde dehydrogenase (ALDH). Subsequently, HCOOH is converted to H-2 by a new iridium polymer complex catalyst and an enzyme mimic is used to convert NADH to H-2 and nicotinamide adenine dinucleotide (NAD(+)). NAD(+) can then be reconverted to NADH by repeating the dehydrogenation of methanol. This strategy and the catalysts invented in this research can also be applied to hydrogen production from other small organic molecules (e.g. ethanol) or biomass (e.g. glucose), and thus will have a high impact on hydrogen storage and applications.
引用
收藏
页码:7498 / 7504
页数:7
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