Graphdiyne Interface Engineering: Highly Active and Selective Ammonia Synthesis

Abstract

A freestanding 3D graphdiyne–cobalt nitride (GDY/Co2N) with a highly active and selective interface is fabricated for the electrochemical nitrogen reduction reaction (ECNRR). Density function theory calculations reveal that the interface‐bonded GDY contributes an unique p‐electronic character to optimally modify the Co‐N compound surface bonding, which generates as‐observed superior electronic activity for NRR catalysis at the interface region. Experimentally, at atmospheric pressure and room temperature, the electrocatalyst creates a new record of ammonia yield rate (YNH3 ) and Faradaic efficiency (FE) of 219.72 μg h−1 mgcat.−1 and 58.60 %, respectively, in acidic conditions, higher than reported electrocatalysts. Such a catalyst is promising to generate new concepts, new knowledge, and new phenomena in electrocatalytic research, driving rapid development in the field of electrocatalysis.

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.…”

Photoinduced Electrocatalysis on 3D Flexible OsOx Quantum Dots

“…The presence of the π–π* transition peak verifies the interaction between OsO x and GDY. [ 28 ] The Os 4f XPS spectrum for the OsO x QDs/GDY (Figure 3d) and OsO x /CC(Figure 3d) shows four characteristic peaks at 51.3, 52.8, 54.1, and 55.5 eV, respectively, indicating the presence of Os 3+ and Os 4+ . The subpeaks at 45.5 and 57.1 eV corresponding to Os 5p 3/2 and Os 5p 1/2 , respectively (Figure 3d,e).…”