Atomic Bridging of Metal‐Nitrogen‐Carbon toward Efficient Integrated Electrocatalysis

Abstract

The rational design of robust electrocatalysts for efficient integrated devices is crucial to enhance energy conversion performance. The coordination of organic ligands with metal ions provides high flexibility to anchor metal atoms among carbon materials. Herein, the atomic anchoring of Zn and Ni atoms into N‐doped carbon networks with adjustable atomic structure is developed by the facile pyrolysis of metal‐organic framework nanoplates in the presence of dicyandiamide. Theoretical calculations reveal the descriptor‐based design principles to adjust the bridging structures of metal‐nitrogen‐carbon moieties with changing d‐band centers, thereby improving electrocatalytic performance. The resulting electrocatalyst displays good multiple electrocatalytic activities for carbon dioxide reduction, oxygen reduction, and evolution reactions, enabling the fabrication of integrated energy devices. Importantly, the CO2‐H2O overall splitting with the as‐prepared electrocatalysts has been driven by the commercial solar cell and the zinc‐air battery assembled with the same catalyst respectively, showing high CO faradaic efficiency up to 90%. Especially, the overall solar‐to‐CO conversion efficiency is up to 13% and the corresponding utilization efficiency of solar‐to‐electricity can reach 54.4%, demonstrating the large promising space to chase the limit that solar cells can possibly achieve. This work provides new opportunities to modulate the atomic bridging structure of metal‐nitrogen‐carbon for integrated electrolysis.

Heteroatom Doped Amorphous/Crystalline Ruthenium Oxide Nanocages as a Remarkable Bifunctional Electrocatalyst for Overall Water Splitting

“…[ 24 ] From Nyquist plots of EIS measurement, Co‐ZnRuO x nanocages display a smaller semicircle diameter than commercial RuO 2 and ZnRuO x nanocages, implying the faster charge transfer between the electrodes and the electrolyte (Figure 4d). [ 25 ] A double‐layered capacitance ( C dl ) measurement was made in a non‐Faradaic potential region to look into the cause of the improvement in OER performance. The high OER intrinsic catalytic activity of Co‐ZnRuO x nanocages is demonstrated by the C dl values of 48.07 mF cm −2 for Co‐ZnRuO x nanocages, 5.25 mF cm −2 for ZnRuO x nanocages, and 12.44 mF cm −2 for commercial RuO 2 (Figure 4e; Figure S12, Supporting Information).…”

Single‐atom electrocatalysts for lithium–sulfur chemistry: Design principle, mechanism, and outlook

“…For this reason, the combination of double and triple SACs might be promising for accelerated redox kinetics and improved efficiency of advanced LSBs. For instance, the synergy of Zn–Ni, 127 Ru–Co, 128 Ni–Cu, 129 Ru–Ni, 130 and Co–Te diatomic sites 131 has led to tunable electron structures in other electrocatalytic systems, which may also be extended to the LSB field for performance enhancement. In this regard, the emerging d‐p orbital hybridization principle can guide the rational construction of SACs.…”

Unraveling the amine oxidative coupling activity of hierarchical porous Fe–N4–O1 single-atom catalysts: oxygen atom-mediated dual reaction pathway

“…S4 †). 25,[37][38][39] Compared with that in Fe-NC (Fig. 2f), the Fe(-N-)C coordination peak in Fe-NC-R (Fig.…”