Facet-Engineering of Materials for Photocatalytic Application: Status and Future Prospects

Ca2+ doped Metal Organic Frameworks for Enhanced Photocatalytic Ammonia Synthesis

The conventional Haber–Bosch NH3 synthesis process requires high temperatures and pressures, resulting in a high carbon footprint and the need to develop alternative NH3 synthesis methods. Accordingly, plasma-based and γ-Al2O3-catalyzed NH3 synthesis from H2O (a hydrogen source) and air/N2 (a nitrogen source) was studied under low temperature and low pressure conditions. The experimental results show that NH3 can be synthesized with air/N2 and H2O, although byproducts such as NO and N2O are also formed. The NH3 formation rate resulting from the use of N2 and H2O is higher than that of air and H2O. Increasing specific energy input (SEI) can increase the NH3 formation rate. Nevertheless, the energy efficiency of NH3 synthesis technology first increases and then decreases with SEI. An NH3 formation rate of 2.92 μmol h–1 g–1 was achieved with an SEI of 11.68 J mL–1 and energy efficiency of 5.10 mg kW–1 h–1 (1.28 mg kWh–1g–1), when wet air at a flow rate of 200 mL min–1 was introduced into the dielectric barrier discharge (DBD) reactor, which was lower than that (4.30 μmol h–1 g–1) attained with N2 + H2O under an SEI of 11.50 J mL–1 and energy efficiency of 7.63 mg kW–1 h–1 (1.91 mg kWh–1g–1). Additionally, the γ-Al2O3 catalyst exhibited good stability. Different results show that plasma-based and γ-Al2O3 catalyzed NH3 synthesis technology is promising. 

One-Step Synthesis of Ammonia Directly from Wet Air/N2 by Plasma Combined with a γ-Al2O3 Catalyst

Ammonia, a pivotal chemical feedstock and a potential hydrogen energy carrier, demands efficient synthesis as a key step in its utilization. The traditional Haber-Bosch process, known for its high energy consumption, has spurred researchers to seek ammonia synthesis under milder conditions. Advances in surface science and characterization technologies have deepened our understanding of the microscopic reaction mechanisms of ammonia synthesis. This article concentrates on gas-solid phase ammonia synthesis, initially exploring the latest breakthroughs and improvements in thermal catalytic synthesis. Building on this, it especially focuses on emerging external field-driven alternatives, such as photocatalysis, photothermal catalysis, and low-temperature plasma catalysis strategies. The paper concludes by discussing the future prospects and objectives of nitrogen fixation technologies. This comprehensive review is intended to provide profound insights for overcoming the inherent thermodynamic and kinetic constraints in traditional ammonia synthesis, thereby fostering a shift towards "green ammonia" production and significantly reducing the energy footprint.

Recent Advances in Ammonia Synthesis: From Haber-Bosch Process to External Field Driven Strategies.

Nonoxidative conversion of methane (NOCM) under mild conditions is a highly desirable technology for the low-carbon and atom-economical production of H2 and value-added chemicals. Here, we report the fabrication of CeO2 nanoisland patterns on the surface of Ce–Zr solid solutions. These ultrasmall CeO2 nanoislands with abundant step-edge structures provide unprecedented methane adsorption and activation, achieving the highest methane conversion rate of 1517 μmol g–1 h–1 for photocatalytic NOCM to date. Density functional theory calculations revealed that the low-coordinated Ce–O units at the stepped CeO2(111) surface possess more open planar configurations, which facilitate the cleavage of methane C–H bonds via a distinct metal–CH4 σ-complex mechanism that is energetically more favorable than the radical-like mechanism on the flat CeO2(111) surface. Moreover, the photocatalyst demonstrated a reversible and cooperative photoactivation process that enables the transition from the “resting state” to the “active state”, thereby enhancing the photoexcited charge separation efficiency and photocatalytic NOCM activities. 

Fabrication of Stepped CeO2 Nanoislands for Efficient Photocatalytic Methane Coupling

Electronic and Interface Regulation of Wurtzite Surfaces Promotes Photocatalytic Ammonia Synthesis under Visible Light Irradiation

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Electronic and Interface Regulation of Wurtzite Surfaces Promotes Photocatalytic Ammonia Synthesis under Visible Light Irradiation