Imaging a Haber-Bosch catalysis precursor at the atomic scale
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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Sustainable ammonia synthesis from nitrogen wet with sea water by single-step plasma catalysis
Ammonia synthesis at ambient conditions employing intermittent distributed green sources of energy and feedstocks is globally sought to replace the centralized Haber-Bosch (H-B) process operating at high temperature and pressure. We report herein for the first time an effective and sustainable ammonia synthesis pathway from N 2 wet with seawater vapor over spherical SiO 2 and M/SiO 2 (M: Ag, Cu, and Co) catalysts driven by non-thermal plasma (NTP). Experimental results indicate that the presence of a catalyst is required for ammonia production from seawater vapor and N 2 . The Co/SiO 2 catalyst delivered the highest ammonia synthesis rate (r NH 3 ) of 3.7 mmol g cat -1 h -1 and energy yield of 3.2 g NH 3 ∙kW -1 ∙h -1 at a relatively low input power of 2 W. The extraction of H atoms from H 2 O molecules plays an important role in the ammonia synthesis from seawater vapor. Finally, this work unfolds a novel platform for the subsequent optimization of sustainable ammonia production from endless resources such as seawater and N 2 through catalytic non-thermal plasma potentially powered by renewable sources.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Gamma Driven Catalysis of Ammonia
Experiments were conducted to investigate a passive production mechanism for the world’s most energy intensive commodity, ammonia. A novel method, gamma catalyzed ammonia production at ambient conditions, was investigated. Ammonia is currently produced through the highly energy intensive Haber-Fritz process, which requires an operation pressure of 400 atmosphere and 600 degrees Celsius. Due to the high demand and need for ammonia, the Haber-Bosch process consumes 25% all energy produced globally. Reported herein was an attempt to produce ammonia at ambient temperature (20 C) and ambient pressure (1 atm), through a novel process developed at PNNL, gamma driven catalysis of ammonia. Although the measurements of the ammonia production suggest wild success, reports in the literature by Gao et.al. suggest an experimental positive bias in the results. To rule out the potential positive bias, multiple additional production campaigns would be needed to with an alternate analysis technique such as ion chromatography, as suggested by Gao et.al. Unfortunately, due to this late determination of potential positive bias, the results of this study remain inconclusive to the feasibility of gamma driven catalysis of ammonia and more work is needed to describe the chemical evolution with time. The results are a first step and demonstrate that gamma-catalyst mediated reactions are possible. This represents a key opportunity to explore the fundamental chemistry of high band gap catalysts that can change the paradigm of radiation, transforming it from a waste to a valuable energy source.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Microwave-enhanced catalytic ammonia synthesis under moderate pressure and temperature
In this study, an alternative approach based on microwave-enhanced ammonia synthesis for Haber-Bosch process was carried out under moderate pressure of 0.1–0.65 MPa and temperature range of 280–400 °C over a stable CsRu/CeO 2 catalyst. The ammonia production rate is significantly improved under microwave conditions. At 0.65 MPa and 320 °C, maximum ammonia production rate was achieved at H 2 /N 2 ratio of 1/1. Stable performance was obtained in a 6-cycles of startup-shutdown operation for cumulative on-line time of 80 h. The work demonstrates the potential of microwave catalytic technology for the distributed ammonia synthesis using renewable power having intermittent nature of energy supply.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Enhancing Nitrogen Activation in Electrochemical Reduction: The Role of Rare Earth Oxide Surface Configurations
The pursuit of sustainable ammonia synthesis has prompted the exploration of ambient electrochemical nitrogen reduction reaction (e-NRR) as an alternative to the energy-intensive Haber-Bosch process. Here, this study conducted a theoretical investigation into the use of rare earth oxide materials, specifically dysprosium oxide (Dy 2 O 3 ), as potential electrocatalysts for NRR. Utilizing spin-polarized density functional theory calculations, we explored the interaction between Dy 2 O 3 surfaces and nitrogen (N 2 ) molecules, examining the capability of Dy 2 O 3 to adsorb and activate N 2 under ambient conditions. The results indicate that Dy 2 O 3 surfaces exhibit diverse configurations and bonding environments, providing a variety of reactive sites that display different behaviors in N 2 adsorption and activation. The distinctive electronic structure and surface chemistry of a particular Dy 2 O 3 surface configuration were found to significantly enhance the activation of N 2 by promoting charge transfer, which facilitates the NRR process. This research provides deep insights into the mechanistic pathways of N 2 reduction over Dy 2 O 3 , highlighting the surface properties as pivotal in catalysis. These theoretical insights serve as a foundation for the development of novel rare earth-based electrocatalytic materials for efficient ambient e-NRR, potentially transforming ammonia production into a greener and more energy-efficient process.
32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
Microwave-Mediated ammonia synthesis over Co 2 Mo 3 N catalysts at low pressures
The Haber-Bosch process for ammonia (NH 3 ) synthesis is a major contributor to greenhouse gas emissions and is responsible for > 2 % of the world’s energy consumption each year encouraging the need for alternative renewable-based options. Here, this study investigates an earth-abundant ternary metal nitride (i.e., Co 2 Mo 3 N) catalyst to develop a renewable-based NH 3 synthesis approach, utilizing an energy-efficient microwave-assisted route. Using a combination of spectroscopic and catalytic measurements coupled with surface analysis techniques, Co 2 Mo 3 N was evaluated as a stable and efficient NH 3 synthesis catalyst. Results presented here demonstrate NH 3 synthesis on Co 2 Mo 3 N at ~420 °C and ambient pressure yield ~0.7 mmolNH3.g cat -1 .h -1 and up to ~12 mmol NH3 .g cat -1 .h -1 at 28 bar under microwave irradiation. Co 2 Mo 3 N displayed an activation energy of ~72 kJ.mol -1 and yielded NH 3 following first-order kinetics with respect to both H 2 and N 2 . These studies illustrate the potential of using this catalyst for a sustainable, cost-effective, and environmentally friendly approach to producing NH 3 .
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Earth-Abundant Manganese Nitride Catalysts for Mild-Condition Ammonia Synthesis
Developing advanced catalytic materials for mild-condition ammonia (NH 3 ) synthesis is essential for improving the energy efficiency of the industrial Haber-Bosch process. Here, in this study, we report a ζ-phase manganese nitride (MnN 0.43 ) catalyst for low-temperature NH 3 synthesis. The as-synthesized MnN 0.43 catalyst is protected by a carbon shell, allowing for the storage and processing of the air-sensitive metal nitride under ambient conditions. After activation in situ, the MnN 0.43 catalyst exhibits high activity for NH 3 synthesis at 250–350 °C, surpassing the conventional noble metal based Ru/MgO catalyst. A combination of kinetic, chemisorption, isotope labeling and computational studies indicate that a nitrogen vacancy-mediated associative mechanism accounts for the catalytic enhancements. Our work highlights the great potential of earth-abundant transition metal nitrides for catalyzing mild-condition NH 3 synthesis.
36 MATERIALS SCIENCE↗