Beyond the Thermal Equilibrium Limit of Ammonia Synthesis with Dual Temperature Zone Catalyst Powered by Solar Light

Mao, Chengliang; Li, Hao; Song, Baokun; Wang, Jiaxian; Zou, Yunjie; Qi, Guodong; Xu, Jun; Shen, Wenjuan; Li, Jie; Liu, Shiyuan; Zhao, Jincai; Zhang, Lizhi

doi:10.1016/j.chempr.2019.07.021

Cited by 126 publications

(90 citation statements)

References 67 publications

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“…5a) attributed to an N-H stretching mode (n N-H ) gradually increases, followed by the increased peaks at 3527 cm À1 assigned to the O-H stretching (n TiO-H ) mode aer water supply. 46 As a result, in situ measurements elucidate that inert N^N is efficiently activated on phase-selective defect sites on Na-A d /R o under 1 sun irradiation, leading to the subsequent N^N cleavage to NH 3 or NH 4 + at the last step.…”

Section: Proposed Mechanistic Pathway For N 2 Xationmentioning

confidence: 95%

Phase-selective active sites on ordered/disordered titanium dioxide enable exceptional photocatalytic ammonia synthesis

et al. 2021

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Section: Proposed Mechanistic Pathway For N 2 Xationmentioning

confidence: 95%

Phase-selective active sites on ordered/disordered titanium dioxide enable exceptional photocatalytic ammonia synthesis

et al. 2021

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“…Recently, an ''equilibrium-beyond'' reactivity was reported for ammonia synthesis using plasmon-based dual-temperature-zone catalysis (Figure 2C2). 45 Finally, coexistence of multi-effects is an important feature of PMCR, as is the fact that these effects often act synergistically with each other. For example, SPs are sensitive to the change in refractive index of its surrounding medium and the density of state of plasmonic nanomaterials; thus, the adsorption or reaction of molecule on the plasmonic nanostructures can change the plasmonic spectrum.…”

Section: Ll Unique Features Of Pmcrmentioning

confidence: 99%

“…Under illumination, plasmonic heating of metallic Fe nanonecklace induces local temperature difference, rendering N 2 activation on high-temperature Fe (red; zone I) and NH 3 generation on low-temperature TiO 2Àx H y (blue; zone II), which leads to the ''equilibrium-beyond'' reactivity. Reprinted from Mao et al,45 with permission. Copyright 2019, Elsevier Inc.…”

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confidence: 99%

Recent Progress and Prospects in Plasmon-Mediated Chemical Reaction

Zhan

Moskovits

Zhang

2020

Matter

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Plasmon-mediated chemical reaction (PMCR) is an emerging field of research and development in which chemical reactions are enabled by plasmonic nanomaterials that function as mediators to redistribute and convert photon energy into localized photon, electron, and/or thermal energies. Multiple recent reports have made it a promising approach for facilitating light-driven chemical reactions by utilizing solar energy. Moreover, based on unique properties of plasmonic nanomaterials, PMCR exhibits differences from and potential advantages over traditional thermochemistry, photochemistry, and photocatalysis. However, PMCR still faces challenges such as a far from complete understanding of its operating mechanisms, which contributes to current limitations in reaction efficiency and selectivity. This Perspective aims to be a relatively complete current physicochemical description of PMCR and provides a comprehensive comparison with other reaction systems as well as identifying unique features. Challenges and opportunities are discussed to guide future directions and stimulate the interest of a broad range of scientists with varying backgrounds.

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“…Photocatalytic NRR at higher temperatures (above ambient) offers improved reaction rates, though solar‐to‐chemical conversion efficiencies are still too low to warrant serious industry interest. [ 79 ] This limitations of photocatalysts can be traced to fast recombination of photoexcited charge carriers and the sluggish water oxidation half‐reaction which provides protons for NH 3 synthesis. The specific activity of some electrocatalysts is on the same order of magnitude as thermal catalysts, though the absolute activity and the concentration of ammonia in produced solution are still low (typically <1 ppm).…”

Section: Discussionmentioning

confidence: 99%

The Journey toward Low Temperature, Low Pressure Catalytic Nitrogen Fixation

Shi

Zhang

Waterhouse

et al. 2020

Advanced Energy Materials

158

101

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Ammonia and its derived products are vital to modern societies. Artificial nitrogen fixation to ammonia via the Haber–Bosch process has been employed industrially for over 100 years. However, the Haber–Bosch process is energy intensive and not sustainable in its current form as it uses hydrogen sourced from steam methane reforming to reduce N2. The roadmap to sustainable NH3 production demands the discovery of novel approaches for nitrogen fixation under near ambient conditions that preferably use water as the reducing agent. Over the last decade, great efforts have been made to develop catalysts capable of N2 fixation under mild reaction conditions, using strategies such as low temperature thermal catalysis, nonthermal plasma catalysis, enzymatic catalysis, photocatalysis, and electrocatalysis to generate ammonia and other valuable nitrogen‐containing chemicals. In parallel with catalytic performance studies, researchers have also placed emphasis on the mechanistic understanding of natural and artificial nitrogen fixation catalysts. In this work, the various routes now being explored for nitrogen fixation are summarized. The different dinitrogen activation and hydrogenation pathways are described, whilst describing key advances made to date on the journey toward near ambient ammonia synthesis. Key obstacles that need to be overcome to attract industry interest are also discussed.

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Beyond the Thermal Equilibrium Limit of Ammonia Synthesis with Dual Temperature Zone Catalyst Powered by Solar Light

Cited by 126 publications

References 67 publications

Phase-selective active sites on ordered/disordered titanium dioxide enable exceptional photocatalytic ammonia synthesis

Phase-selective active sites on ordered/disordered titanium dioxide enable exceptional photocatalytic ammonia synthesis

Recent Progress and Prospects in Plasmon-Mediated Chemical Reaction

The Journey toward Low Temperature, Low Pressure Catalytic Nitrogen Fixation

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