2019
DOI: 10.1021/acsenergylett.9b00860
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Light-Driven Chemical Looping for Ammonia Synthesis

Abstract: Synthetic ammonia has been the primary worldwide source of agricultural fertilizer over the last century and is a promising carbon-free energy carrier for sustainable transportation. Despite its global importance, synthetic ammonia produced with the Haber−Bosch process is extremely energy-and resource-intensive. Here we demonstrate a three-step chemical looping strategy to produce ammonia using only light, natural gas, nitrogen, and water. Titanium nitride nanoparticles were utilized as plasmonic antennas to a… Show more

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Cited by 88 publications
(75 citation statements)
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“…One year later, Halas and co-workers published another paper in the same field, and they demonstrated an innovative route to produce ammonia using titanium nitride NPs as plasmonic antennas, which can heat magnesium-based nanomaterials to undergo chemical looping as active materials. 251 The researchers manufactured a customized low-pressure reaction chamber to perform the three-step chemical looping process and to monitor the product formation in situ via isotopic labelling and rotational spectroscopy. During the experiment, the catalytic system was irradiated with a Ti:sapphire laser (808 nm wavelength, 150 fs pulses, 80 MHz repetition rate) with different timing for each step.…”
Section: Nh 3 Synthesis/decompositionmentioning
confidence: 99%
“…One year later, Halas and co-workers published another paper in the same field, and they demonstrated an innovative route to produce ammonia using titanium nitride NPs as plasmonic antennas, which can heat magnesium-based nanomaterials to undergo chemical looping as active materials. 251 The researchers manufactured a customized low-pressure reaction chamber to perform the three-step chemical looping process and to monitor the product formation in situ via isotopic labelling and rotational spectroscopy. During the experiment, the catalytic system was irradiated with a Ti:sapphire laser (808 nm wavelength, 150 fs pulses, 80 MHz repetition rate) with different timing for each step.…”
Section: Nh 3 Synthesis/decompositionmentioning
confidence: 99%
“…Transmission electron microscopy will continue to play an important role in catalyst development. Optically coupled electron microscopy will undoubtedly play an essential role in understanding the effect of light on many other phase-transformations beyond hydrides, such as oxides and nitrides . The integration of additional analytical techniques in the electron microscope such as electron- and light-stimulated Raman spectroscopy (ELISR), mass spectrometry, and ultrasensitive gas-phase molecular spectroscopy , will be an important addition to our analytical toolbox as we seek to understand photocatalysts with high spatial and chemical resolution.…”
Section: Discussionmentioning
confidence: 99%
“…Optically coupled electron microscopy will undoubtedly play an essential role in understanding the effect of light on many other phase-transformations beyond hydrides, such as oxides 56 and nitrides. 57 The integration of additional analytical techniques in the electron microscope such as electron-and light-stimulated Raman spectroscopy (ELISR), 58 mass spectrometry, 59 and ultrasensitive gas-phase molecular spectroscopy 60,61 will be an important addition to our analytical toolbox as we seek to understand photocatalysts with high spatial and chemical resolution. Finally, given the subpicosecond timescales of plasmonic excitation and excitedstate chemistry, the next generation of ultrafast electron microscopes will play an increasingly vital role in characterizing optically driven processes at the single-and subparticle levels.…”
Section: Discussionmentioning
confidence: 99%
“…Chemical looping processes are a promising route for improving energy efficiency, [1][2][3][4] leveraging renewable energy sources, [5][6][7][8][9][10][11] facilitating chemical conversions, [12][13][14][15][16][17][18][19][20] and reducing undesirable emissions across many sectors of the chemical industry. [21][22][23][24][25][26] In a chemical looping (CL) process, the overall reaction is separated into multiple (typically two) subreactions, each mediated by the redox chemistry of a "looped" active material.…”
Section: Introductionmentioning
confidence: 99%