First principles and machine learning based superior catalytic activities and selectivities for N₂ reduction in MBenes, defective 2D materials and 2D π-conjugated polymer-supported single atom catalysts

Abstract

The catalytic activity and selectivity can be improved for nitrogen fixation by using hollow sites and vacancy defects in 2D materials, while a new machine learning descriptor accelerates screening of efficient electrocatalysts.

Mutual modulationviacharge transfer and unpaired electrons of catalytic sites for the superior intrinsic activity of N2reduction: from high-throughput computation assisted with a machine learning perspective

“…22 With the inspiration and opportunities presented by machine learning (ML), a number of related studies using ML-assisted methods have emerged for the prediction of the formation energy of crystals, 23 superhard compounds 24 and catalytic activity. [25][26][27][28][29][30][31] In general, material features should be properly selected for descriptor-to-property mapping in ML.…”

“…27 Substitutional doping of boron can largely retain the host lattice unchanged and simultaneously induce tailored electronic structure, which triggers the catalytic activity. 28,29,43,44 Kumar et al demonstrated that using boron-doped MoS 2 nanosheets is an effective strategy for tailoring the physical properties of MoS 2 and successfully fabricated them through experiments. 43 Li et al showed that di-boron pair doped MoS 2 monolayer exhibits superior catalytic activity for NRR by rst-principles simulations.…”

“…Recently, data-driven method brought about great success in computer vision 20 , natural language processing 21 and speech recognition 22 . With the inspiration and opportunities of machine learning (ML), amounts of related studies using MLassisted method have emerged for prediction of formation energy of crystals 23 , superhard compounds 24 and catalytic activity [25][26][27][28][29][30][31] . In general, material features should be properly selected for descriptor-to-property mappings in ML.…”

“…The boron can not only be active anchoring site but also substitutional doped element into the substrate 27 . Substitutional doping of boron can largely retain the host lattice unchanged and simultaneously 4 induce tailored electronic structure which triggers the catalytic activity 28,29,43,44 . Kumar et al demonstrated that boron-doped MoS 2 nanosheet is an effective strategy for tailoring the physical properties of MoS 2 and fabricated it successfully in experiment 43 .…”

Theoretical investigation on hydrogenation of dinitrogen triggered by singly dispersed bimetallic sites

“…The adsorption of the N 2 molecule on SCCs is vital to activate the inert N^N triple bond, and also meaningful for subsequent hydrogenation. 43 Owing to the low oxidation state of the doped metals in the stable M 1 Co n /CoO x SCCs (M ¼ Ni, Cu, Ru, Rh, Pd, Ag, Os, Ir, Pt, Au), the isolated bimetallic sites have the potential to enhance the chemisorption of N 2 to effectively activate the N^N triple bond.…”