Fe-Doped 1T/2H Mixed-Phase MoS₂/C Nanostructures for N₂ Electroreduction into Ammonia

Abstract

Recently, molybdenum (Mo)-based catalysts have been proved to be effective NRR catalysts due to the high affinity of nitrogen to Mo. The design of a heterostructure and the introduction of defects, such as vacancies and heteroatom doping, are effective means to regulate the microstructure of catalysts and further improve their electrocatalytic N2 into NH3 performance. In this paper, VS-Fe-doped 1T/2H mixed-phase MoS2/C (VS means sulfur vacancies) heterostructure sphere-like nanoflowers with rich sulfur vacancies are prepared through a pectin-assisted hydrothermal reaction, followed by calcination and treatment with NaBH4 solution. VS-Fe-MoS2/C exhibits good electrocatalytic NRR performance with a high ammonia yield rate of 17.8 ± 0.7 μg h–1 mg–1 at −0.5 V versus reversible hydrogen electrode (vs RHE) and a Faraday efficiency (FE) of 9.2% at −0.3 V (vs RHE) under ambient conditions. Introducing sulfur vacancies, iron doping, and preparing 2H-phase MoS2 have greatly improved the performance of electrocatalytic nitrogen reduction to ammonia.

Co-Doped Fe3S4 Nanoflowers for Boosting Electrocatalytic Nitrogen Fixation to Ammonia under Mild Conditions

“…It has been proved that element doping engineering can not only improve the electronic structure of the catalysts but also introduce extra defects to further improve the catalytic activity. , Co element doping into Fe-based nanomaterials can be an effective way to reasonably modulate the electronic structure of the catalyst due to the smaller atom size and larger electronegativity of the Co atom, as well as the d–d coupling to reduce the free-energy barrier of dissociating the NN triple bond, which has not been explored before. Furthermore, inspired by breakthroughs in morphology engineering, we know that the nanoflower structure itself has a large specific surface area and abundant surface active sites, which can provide more contact sites with electrolytes, promote electron transfer, as well as enhance the performance of electrocatalytic ammonia production. − …”

First-principles-driven catalyst design protocol of 2D/2D heterostructures for electro- and photocatalytic nitrogen reduction reaction

“…On the other hand, if the built-in electric field is in the opposite direction to that of the band alignment, the heterojunction is considered as a direct Z-scheme leading to higher electron and hole potentials at different sides of the heterostructure. For example, 2D/2D Cs 3 Bi 2 Br 9 /CdS 94 for nitrogen fixation, 2D/2D As/ZrS 2 (HfS 2 ) HSs, 98 TiO 2 /h-BN 160 and GeS/WS 2 156 for water splitting, 2D/2D MoS 2 /BA 2 PbI 4 95 for solar cells, and SnS/(CH 3 NH 3 ) 2 AgBiI 6 161 for CO 2 reduction. From the calculations, the effective mass of carriers for Cs 3 Bi 2 Br 9 /CdS vdWHs is reduced, thus accelerating the carrier transfer and decreasing the probability of carrier recombination.…”

Chemical Looping Ammonia Synthesis with High Performance Supported Molybdenum-based Nitrogen Carrier

“…钼基氨合成催化剂 [23][24][25][26][27] , 如过渡金属氮化物 Mo 2 N 因其良好的选择性及活性而被广泛应用于催化合成氨 领域 [28] . 由于 Mo 2 N 催化剂在固氮生成氨的过程中遵循 Mars-van Krevelen 机制 [29] , 该机制涉及氮空位的消耗及 补充, 这与化学链合成氨过程中的释氮及固氮过程有较 强的相似性.…”