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The preparation of formic acid by direct reduction of carbon dioxide is an important basis for the future chemical industry and is of great significance. Due to the serious shortage of highly active and selective electrocatalysts leading to the development of direct reduction of carbon dioxide is limited. Herein the target catalysts with high CO2RR activity and selectivity were identified by integrating DFT calculations and high‐throughput screening and by using graphdiyne (GDY) supported metal oxides quantum dots (QDs) as the ideal model. It is theoretically predicted that GDY supported indium oxide QDs (i.e. InOx/GDY) is a new heterostructure electrocatalyst candidate with optimal CO2RR performance. The interfacial electronic strong interactions effectively regulate the surface charge distribution of QDs and affect the adsorption/desorption behavior of HCOO* intermediate during CO2RR to achieve highly efficient CO2 conversion. Based on the predicted composition and structure, we synthesized the advanced catalytic system, and demonstrates superior CO2‐to‐HCOOH conversion performance. The study presents an effective strategy for rational design of highly efficient heterostructure electrocatalysts to promote green chemical production. [ABSTRACT FROM AUTHOR]

The lack of highly active and selective catalysts is a major obstacle to replace traditional Haber–Bosch process for electrocatalytic production of ammonia (NH3) at ambient conditions. A new hollow graphdiyne nanoreactor (GDYNR) is reported to overcome this issue effectively. The GDYNR is synthesized by in situ growth of GDY on the inner and outer surfaces of the cobalt hydroxide sphere to form a high‐performance interface structure. Experimental results demonstrate that the incomplete charge transfer between GDY and cobalt atoms at the interfaces promotes the formation of strong interfacial sp‐C─Co bonds and the transition of monovalent Co(II) to mixed Co(II)/Co(III) phases. These intrinsic characteristics give the GDYNR superior NH3 production performances with the highest NH3 yield rate (YNH3) of 479 830.67 µgNH3 mgcat−1 h−1, Faradaic efficiency (FE) of ≈100% at −0.4 V versus reversible hydrogen electrode, and excellent long‐term stability at room temperatures and ambient pressures, along with no side reactions. In light of characteristics of the unique confined hollow structures and the heterointerface with obvious incomplete charge transfer property, the generation of GDYNR system represents an advanced design concept and preparation technology for the development of catalytic systems with new structures. [ABSTRACT FROM AUTHOR]

The development of new catalysts with high selectivity and efficiency for the electrocatalytic nitrate reduction reaction (NtRR) to produce ammonia (NH3) at room temperature and ambient pressure is still a challenge. Herein, we report a simple in situ growth method for the controlled synthesis of a GDY–MnOx heterointerface by selectively anchoring and growing MnOx on GDY surfaces. Experimental results show that the incomplete charge-transfer between GDY and Mn atoms at the interface structures largely increases the number of active sites, improves the electrical conductivity, and therefore results in excellent electrocatalytic performance for NH3 synthesis with a maximum FE of 95.4%, an NH3 yield rate of 463.4 μmol h−1 cm−2 and high long-term stability in 0.1 M KOH + 0.1 M NO3− aqueous electrolytes at room temperature and ambient pressure. [ABSTRACT FROM AUTHOR]

Water electrolysis provides an effective method for energy efficient hydrogen production. The challenge in this field is how to synthesize electrocatalysts with high activity and stability in water electrolysis reactions. Herein, a new heterostructure of graphdiyne-iron oxyhydroxide was synthesized by controlled growth of GDY films on the surface of FeOOH nanowires (FeOOH@GDY). An interface structure with an electron-donor (GDY) and electron-acceptor (Fe) was formed, which showed the obvious incomplete charge transfer between GDY and Fe atoms at the interfaces. This produces infinite active sites which guarantee excellent catalytic activity. The GDY grown on the surfaces of oxyhydroxides endows the electrocatalyst with high stability. These unique and fascinating properties make FeOOH@GDY show excellent catalytic activities toward overall water splitting (OWS) with a small cell voltage of 1.43 V at 10 mA cm−2 under ambient conditions and excellent long-term stability. [ABSTRACT FROM AUTHOR]