Recent progress in Green Ammonia: Production, applications, assessment; barriers, and its role in achieving the sustainable development goals

Plasma catalysis is gaining increasing interest for various applications, but the underlying mechanisms are still far from understood. Hence, more fundamental research is needed to understand these mechanisms. This can be obtained by both modelling and experiments. This foundations paper describes the fundamental insights in plasma catalysis, as well as efforts to gain more insights by modelling and experiments. Furthermore, it discusses the state-of-the-art of the major plasma catalysis applications, as well as successes and challenges of technology transfer of these applications.

Foundations of plasma catalysis for environmental applications

: Plasma-based ammonia synthesis is studied as an option for electrifying the chemical industry. However, the energy e ﬃ ciency of plasma-based ammonia synthesis is severely limited by ammonia decomposition in the plasma phase. We show that the use of zeolite 4A as an adsorbent for in situ ammonia removal from the plasma phase suppresses product decomposition, thereby increasing the ammonia yield. It is found that the ammonia yield for plasma-chemical ammonia synthesis with in situ ammonia removal is improved by a factor of 2 compared to steady-state plasma-chemical ammonia synthesis. Plasma-induced surface heating limits the e ﬀ ective ammonia adsorption capacity of the zeolite, decreasing the adsorption capacity. In situ product removal is of interest for plasma chemistry and plasma catalysis, in general, as the product decomposition in the plasma is a general phenomenon limiting the product yield.

/pdf/improving-the-energy-yield-of-plasma-based-ammonia-synthesis-hqo2v95e.pdf

Improving the Energy Yield of Plasma-Based Ammonia Synthesis with In Situ Adsorption

Plasma-assisted catalysis is emerging as an alternative to several thermocatalytic processes. For ammonia synthesis, it could make the process milder, which would help production, decentralization, and compatibility with renewable energy. However, one major obstacle preventing optimization of the plasma-assisted process is the incipient mechanistic understanding of ammonia formation on plasma-exposed catalysts. Here, optical emission spectroscopy is consistent with only a weak effect of the metal on plasma composition and with the presence of small concentrations of plasma radicals in N2/H2 mixtures in dielectric barrier discharge (DBD) reactors, which are bound to enable new catalyst-involved pathways not considered in previous kinetic models for NH3 synthesis. Thus, we comprehensively examined, via density functional theory calculations, the energetics (favorability) of 51 reactions on Fe, Ni, Co, Pd, Ga, Sn, Cu, Au, and Ag. Enthalpic barriers for Eley–Rideal (ER) reactions involving N• and H• radicals were found to be negligible and hence supportive of the following: (i) plausible NNH formation and consequent prominent role of the associative pathway to form NH3 (consistent with some experimental reports detecting surface-bound NXHY species), (ii) likelihood of N• adsorption taking over N2* dissociation as the primary source of surface bound N*, and (iii) probable dominance of ER hydrogenation reactions over Langmuir–Hinshelwood ones. The energetics herein presented will allow thoroughly studying the pathway competition in future kinetic models, but numbers calculated here already suggest that the dominant pathway may change with the metal identity. For instance, N2HY dissociation favorability is more likely to become competitive with ER hydrogenation earlier in the hydrogenation sequence the more nitrophilic the metals. Yet, the calculated favorability of ER reactions is also already consistent with the weaker dependence of initial NH3 turnover frequencies (TOFs) on metal identity compared to the thermocatalytic scenario. With practical implications for computational catalyst screening, TOFs experimentally measured herein for an atmospheric DBD reactor linearly correlate with ΔErxn for the ER hydrogenation reaction H• + HNNH2* → HNNH3*. This descriptor may be robust to exact synthesis conditions, as its correlation with TOFs was maintained for earlier TOF data in a sub-atmospheric radio frequency reactor. 

Energetics of Reaction Pathways Enabled by N and H Radicals during Catalytic, Plasma-Assisted NH3 Synthesis

Is a catalyst always beneficial in plasma catalysis? Insights from the many physical and chemical interactions

https://pubs.rsc.org/en/content/articlepdf/2021/cy/d0cy02189j

Plasma-catalytic ammonia synthesis beyond thermal equilibrium on Ru-based catalysts in non-thermal plasma

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Plasma-catalytic ammonia synthesis beyond thermal equilibrium on Ru-based catalysts in non-thermal plasma