Highly efficient and highly selective CO2 reduction to CO driven by laser

Yan, Bo; Li, Yinwu; Cao, Wenwu; Zeng, Zhiping; Liu, Pu; Ke, Zhuofeng; Yang, Guowei

doi:10.1016/j.joule.2022.11.005

Cited by 19 publications

(15 citation statements)

References 36 publications

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“…Many energetically active particles react with each other quickly inside the cavitation bubbles. During the rapid quenching process, the reaction is cooled quickly, and the small bubbles finally collapse and release the final products …”

Section: Resultsmentioning

confidence: 99%

Efficient and Rapid Hydrogen Extraction from Ammonia–Water via Laser Under Ambient Conditions without Catalyst

Yan,

Li,

Cao

et al. 2024

J. Am. Chem. Soc.

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As a good carrier of hydrogen, ammonia–water has been employed to extract hydrogen in many ways. Here, we demonstrate a simple, green, ultrafast, and highly efficient method for hydrogen extraction from ammonia–water by laser bubbling in liquids (LBL) at room temperature and ambient pressure without catalyst. A maximum apparent yield of 33.7 mmol/h and a real yield of 93.6 mol/h were realized in a small operating space, which were far higher than the yields of most hydrogen evolution reactions from ammonia–water under ambient conditions. We also established that laser-induced cavitation bubbles generated a transient high temperature, which enabled a very suitable environment for hydrogen extraction from ammonia–water. The laser used here can serve as a demonstration of potentially solar-pumped catalyst-free hydrogen extraction and other chemical synthesis. We anticipate that the LBL technique will open unprecedented opportunities to produce chemicals.

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Section: Resultsmentioning

confidence: 99%

Efficient and Rapid Hydrogen Extraction from Ammonia–Water via Laser Under Ambient Conditions without Catalyst

Yan,

Li,

Cao

et al. 2024

J. Am. Chem. Soc.

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“…Therefore, in 1 h (no laser; dark time, 1 h–0.36 ms), the actual working time of the laser is only 0.36 ms (light time), and the amount of 44.07 mg/L can be produced. If the laser frequency can be greatly increased, which can greatly improve the light time of laser action and reduce the dark time, more microbubbles can be generated . This would lead to a qualitative leap in the yield of HCN, infinitely close to the quasi-continuous laser.…”

Section: Results and Discussionmentioning

confidence: 99%

“…This process is called laser bubbling in liquid (LBL). Like water being decomposed quickly into a nonequilibrium plasma state, LBL would result in the violent decomposition of the molecular structure. − With the laser acting on liquid, a lot of small bubbles of active substances are immediately generated, − and the temperature inside the laser-generated bubble would reach as high as about 10 4 K. , Additionally, a large number of active species (e.g., CH 3 O • ; CH 2 O • ; CH 3 • ; OH • ; H • and N • radicals; and CH 3 O – , CH 2 O – , CH 3 + , OH – , and H + ions) are created inside bubbles. These active substances would be instantaneously activated and cured , to form HCN in the LBL process at high temperatures and with rapid quenching.…”

Section: Introductionmentioning

confidence: 99%

“…If the laser frequency can be greatly increased, which can greatly improve the light time of laser action and reduce the dark time, more microbubbles can be generated. 25 This would lead to a qualitative leap in the yield of HCN, infinitely close to the quasi-continuous laser. As shown in Figure 4D, increasing the frequency of laser and the number of beam-splitting lasers could improve the yield of the production.…”

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confidence: 99%

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Laser-Induced Activation of N₂ and Catalyst-Free Synthesis of HCN

Cao

Liu

et al. 2023

ACS Sustainable Chem. Eng.

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Hydrogen cyanide (HCN) is typically synthesized using ammonia and methane as sources of nitrogen and carbon, respectively, over expensive platinum catalysts at high temperatures. However, continuous high-temperature processing deactivates the catalyst, resulting in limited durability of the process. Besides, there are serious hazards and limitations in the further separation and utilization of HCN. From the perspective of sustainable synthesis and safe utilization, low-cost catalyst or catalyst-free synthesis, mild reaction conditions, and elimination of exposure to toxic reagents are becoming increasingly important. Direct synthesis of HCN from nitrogen (N 2 ) at room temperature without any catalysts and its safe fixation into functional inorganic cyanides are desirable. Here, we report the catalyst-free synthesis of HCN by laser-induced activation of N 2 and methanol (CH 3 OH) at room temperature and then the in situ synthesis of inorganic cyanides (silver and copper cyanides) without purification and separation by reacting the synthetic solution with noble metals. We also establish the possible reaction paths by density functional theory calculations and molecular dynamics simulations to elucidate the thermodynamics and kinetics of the reactions involved in the laser chemistry process, i.e., laser bubbling in liquid (LBL). The high temperature inside the laser-generated bubble overcomes the energy barrier and drives the successful coupling of carbon and nitrogen sources endergonically in the following process. Bubbles experience a rapid quench during the LBL process, resulting in the kinetic control product HCN with high efficiency. The method is viable for the catalyst-free direct synthesis of HCN from N 2 and CH 3 OH at normal conditions for safe fixation into inorganic cyanides.

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“…As thermal energy is being replaced with other types of energy to overcome the activation energy barrier inherent to any chemical transformation, traditional thermal catalysis has been expanded to other types of catalysis such as electrocatalysis, [1][2][3][4][5][6][7][8][9][10][11][12] photocatalysis, 13,14 plasma catalysis, 15,16 and laser catalysis, 17 just to mention a few. This shift, especially to electrocatalysis, is driven by the interest in substituting fossil fuels (which provide heat) with alternative renewable energy sources (like electricity, solar, wind, tidal, etc.).…”

Section: Introductionmentioning

confidence: 99%