Graphdiyne-based metal atomic catalysts for synthesizing ammonia

Abstract

Exploring new catalysts for nitrogen reduction at ambient pressures and temperatures with ultrahigh ammonia (NH3) yield and selectivity is still a giant challenge. In this work, atomic catalysts with separated Pd atoms on graphdiyne (Pd-GDY) have been synthesized and show fascinating electrocatalytic properties for nitrogen reduction. Outstandingly, the catalyst shows the highest average NH3 yield of 4.45 ± 0.30 mgNH3 mgPd−1 h−1, almost tens of orders larger than previously reported ones, and 100% reaction selectivity in neutral media. And Pd-GDY exhibits almost no decreases in the NH3 yield and Faradaic efficiency. Density functional theory calculations show that the reaction pathway prefers to perform at the (Pd, C1, C2) active area due to the strongly coupled (Pd, C1, C2) which elevates the selectivity via enhanced electron-transfer. By adjusting the p-d coupling accurately, the reduction of self-activated nitrogen is promoted by anchoring atom selection, and the side effects are minimized.

Efficient Hydrogen Evolution on Nanoscale Graphdiyne

“…Accordingly, GDY might be expected to realize efficient and effective water splitting without any modification-unique behavior when compared with that of traditional carbon materials. [13][14][15][16][17][18][19][20][21][22][23][24][25][26][27][28][29] In addition, the vertically aligned arrays of GDY should facilitate electron transport and, thus, improve the HER performance. As far as we are aware, however, there have been no previous reports describing the use of GDY as a metal-free catalyst for the HER.…”

Bimetallic Mixed Clusters Highly Loaded on Porous 2D Graphdiyne for Hydrogen Energy Conversion

“…Graphdiyne (GDY), a new 2D carbon allotrope containing sp ‐ and sp 2 ‐hybridized carbon atoms featuring uniformly triangular pores, uneven distribution surface charge, superior electrical conductivity and high stability, has been demonstrated as a promising electrode material applied in numerous fields from catalysis to energy conversion and storage. [ 18 , 19 , 20 , 21 , 22 , 23 , 24 , 25 , 26 , 27 , 28 , 29 , 30 , 31 , 32 , 33 , 34 , 35 , 36 , 37 , 38 , 39 , 40 , 41 , 42 , 43 , 44 , 45 ] The well‐defined porous structure of GDY endow it with numerous unique properties superior to traditional carbon materials. For example, the presence of sp‐C atoms (−C≡C−) in porous GDY leads to the formation of infinite active sites and highly intrinsic activity in catalysis.…”

Adsorption-regulated precise synthesis of atomically-dispersed bimetallic Fe-Co sites on carbon for electrocatalytic nitrogen reduction reaction

“…The experimental system setup and analytical methods are illustrated in Supplementary Figs. [13][14][15][16] and detailed in Method section. The NRR performance of Fe/Co-O-C-1.0 was rstly examined.…”

“…To date, the carbon supported SAECs have been fabricated via two common approaches. One anchors SAs to carbon supports through calcination, while another employs metal ions-impregnated carbonisable precursors to anchor SAs via carbonisation [7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][24][25][26][27] . The former normally involves a simple one-pot synthetic procedure, however, through the calcination process to precisely control SAs loading on a pre-carbonised support is di cult 5,6,19 .…”