Amorphizing of Au Nanoparticles by CeOx–RGO Hybrid Support towards Highly Efficient Electrocatalyst for N2 Reduction under Ambient Conditions

Ammonia synthesis is one of the most kinetically complex and energetically challenging chemical processes in industry and has used the Harber–Bosch catalyst for over a century, which is processed under both harsh pressure (150–350 atm) and hightemperature (623–823 K), wherein the energy and capital intensive Harber–Bosch process has a huge energy cost accounting for about 1%–3% of human's energy consumption. Therefore, there has been a rough and vigorous exploration to find an environmentally benign alternative process. As the amorphous material is in a metastable state and has many "dangling bonds", it is more active than the crystallized one. In this paper, CeO_x-induced amorphization of Au nanoparticles anchored on reduced graphite oxide (a-Au/CeO_x–RGO) has been achieved by a facile coreduction method under ambient atmosphere. As a proof-of-concept experiment, a-Au/CeO_x–RGO hybrid catalyst containing the low noble metal (Au loading is 1.31 wt%) achieves a high Faradaic efficiency (10.10%) and ammonia yield (8.3 μg h⁻¹ mg⁻¹_cat.) at −0.2 V versus RHE, which is significantly higher than that of the crystalline counterpart (c-Au/RGO), and even comparable to the yields and efficiencies under harsh temperatures and/or pressures.

CeO_x-induced amorphization of Au nanoparticles anchored on reduced graphite oxide (a-Au/CeO_x–RGO) as a heterogeneous electrocatalyst shows excellent catalytic activity for electrochemical N₂ reduction reaction with high Faradic efficiency (10.10%) and ammonia yield (8.3 μg h^-1 mg^-1_cat.)

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