A Multi‐Layer Device for Light‐Triggered Hydrogen Production from Alkaline Methanol

Abstract

It usually requires high temperature and high pressure to reform methanol with water to hydrogen with high turnover frequency (TOF). Here we show that hydrogen can be produced from alkaline methanol on al ight-triggered multilayer system with avery high hydrogen evolution rate up to ca. 1 mmol s À1 under the illumination of as tandardP t-decorated carbon nitride.T he system can achieve ar emarkable TOFu p to 1.8 10 6 moles of hydrogen per mole of Pt per hour under mild conditions.T he total turnover number (TTN) of 470 000 measured over 38 hours is among the highest reported. The system does not lead to any CO x emissions,hence it could feed clean hydrogen to fuel cells.Incontrast to aslurry system, the proposed multi-layer system avoids particle aggregation and effectively uses light and Pt active sites.The performance is also attributed to the light-triggered reforming of alkaline methanol. This notable performance is apromising step toward practical light-driven hydrogen generation.

Insight on Reaction Pathways of Photocatalytic CO2 Conversion

“… 74 , 121 We have also recently developed a flow-reactor for oxidative coupling of methane to C 2 products and a multilayer device for methanol reforming. 8 , 122 All these devices for the equivalent photocatalytic reactions might accelerate the development of efficient and scalable devices for practical CO 2 photoconversion, especially driven by the current global concern of the critical climate change.…”

“…The reported examples of such membrane reactors include C 3 N 4 or TiO 2 on Nafion membrane, , TiO 2 on carbon paper, TiO 2 and Cu–TiO 2 on zeolitic imidazolate framework (ZIF-8), and so on, which are good examples for the potential use in a flow system. Reactors under concentrated solar power also have been developed to obtain the high density of electron–hole pairs in the photocatalyst, and the catalyst can also be heated to high temperatures. , We have also recently developed a flow-reactor for oxidative coupling of methane to C 2 products and a multilayer device for methanol reforming. , All these devices for the equivalent photocatalytic reactions might accelerate the development of efficient and scalable devices for practical CO 2 photoconversion, especially driven by the current global concern of the critical climate change.…”

“…Inspired by the fact that the majority of carbon on the Earth’s surface is stored in the form of carbonates, scientists have developed thermodynamically favorable CO 2 -to-carbonate mineralization technologies . Recently, the concept of converting a carbon-containing fuel into carbonates and carbon-free hydrogen was reported . Meanwhile, inspired by natural photosynthesis, scientists have also made significant progress in uphill reactions to fix CO 2 into high-value fuels with the input of energy from sunlight.…”

“…7 Recently, the concept of converting a carbon-containing fuel into carbonates and carbon-free hydrogen was reported. 8 Meanwhile, inspired by natural photosynthesis, scientists have also made significant progress in uphill reactions to fix CO 2 into high-value fuels with the input of energy from sunlight. Such sustainable solar fuels are attractive with a satisfactory density of energy stored in their chemical bonds (e.g., 20 MJ/kg for methanol), which are significantly higher than current batteries (∼0.1−0.7 MJ/ kg) and able to be released on demand without additional carbon emission.…”

Ruthenium Metal–Organic Frameworks as Stable Nanostructures for Selective Hydrogen Production from Acetaldehyde and Water under Mild Conditions

“…Because of their high gravimetric hydrogen content, organic liquids have attracted much interest in hydrogen production and storage. − The hydrogen production contents from methanol, formic acid, and formaldehyde in water are 12, 4.4, and 8.3 wt %, respectively, which have made these C 1 organics research hotspots. − Various catalysts have been developed for selective decompositions of these compounds. The C–H and C–O bonds of these C 1 organics can be activated by catalysts during a hydrogen-releasing process, demonstrating some methods for hydrogen production and storage. , Actually, the relevant C 2 organics have higher gravimetric hydrogen content, higher energy density, and lower damage compared to corresponding C 1 organics. The hydrogen contents of ethanol, acetaldehyde, and acetic acid are up to 13.1, 9.1, and 6.67 wt %, respectively.…”