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Selective two-electron (2e − ) oxygen reduction reaction (ORR) offers great opportunities for hydrogen peroxide (H 2 O 2 ) electrosynthesis and its widespread employment depends on identifying cost-effective catalysts with high activity and selectivity. Main-group metal and nitrogen coordinated carbons (M-N-Cs) are promising but remain largely underexplored due to the low metal-atom density and the lack of understanding in the structure-property correlation. Here, we report using a nanoarchitectured Sb 2 S 3 template to synthesize high-density (10.32 wt%) antimony (Sb) single atoms on nitrogen- and sulfur-codoped carbon nanofibers (Sb-NSCF), which exhibits both high selectivity (97.2%) and mass activity (114.9 A g −1 at 0.65 V) toward the 2e − ORR in alkaline electrolyte. Further, when evaluated with a practical flow cell, Sb-NSCF shows a high production rate of 7.46 mol g catalyst −1 h −1 with negligible loss in activity and selectivity in a 75-h continuous electrolysis. Density functional theory calculations demonstrate that the coordination configuration and the S dopants synergistically contribute to the enhanced 2e − ORR activity and selectivity of the Sb-N 4 moieties. Selective two-electron oxygen reduction reaction is critical electrochemical process for H 2 O 2 electrosynthesis. Here, the authors develop a Sb 2 S 3 -templated strategy to fabricate high-density atomic dispersion of Sb on N,S-codoped hollow carbon nanofiber substrate, which facilitate with the improved selectivity, catalytic mass activity and production rate of H 2 O 2 .

Conversion into high-value-added organic nitrogen compounds through electrochemical C-N coupling reactions under ambient conditions is regarded as a sustainable development strategy to achieve carbon neutrality and high-value utilization of harmful substances. Herein, we report an electrochemical process for selective synthesis of high-valued formamide from carbon monoxide and nitrite with a Ru 1 Cu single-atom alloy under ambient conditions, which achieves a high formamide selectivity with Faradaic efficiency of 45.65 ± 0.76% at −0.5 V vs. RHE. In situ X-ray absorption spectroscopy, coupled with in situ Raman spectroscopy and density functional theory calculations results reveal that the adjacent Ru-Cu dual active sites can spontaneously couple *CO and *NH 2 intermediates to realize a critical C-N coupling reaction, enabling high-performance electrosynthesis of formamide. This work offers insight into the high-value formamide electrocatalysis through coupling CO and NO 2 − under ambient conditions, paving the way for the synthesis of more-sustainable and high-value chemical products. Conversion into high-value-added organic nitrogen compounds through electrochemical C-N coupling reactions is considered a sustainable strategy to achieve carbon neutrality. Herein, we report the selective electrosynthesis of formamide from carbon monoxide and nitrite using Ru 1 Cu single-atoms catalyst.

Lithium‐ion batteries (LIBs) with higher energy density are very necessary to meet the increasing demand for devices with better performance. With the commercial success of lithiated graphite, other graphite intercalation compounds (GICs) have also been intensively reported, not only for LIBs, but also for other metal (Na, K, Al) ion batteries. In this Progress Report, we briefly review the application of GICs as anodes and cathodes in metal (Li, Na, K, Al) ion batteries. After a brief introduction on the development history of GICs, the electrochemistry of cationic GICs and anionic GICs is summarized. We further briefly summarize the use of cationic GICs and anionic GICs in alkali ion batteries and the use of anionic GICs in aluminium‐ion batteries. Finally, we reach some conclusions on the drawbacks, major progress, emerging challenges, and some perspectives on the development of GICs for metal (Li, Na, K, Al) ion batteries. Further development of GICs for metal (Li, Na, K, Al) ion batteries is not only a strong supplement to the commercialized success of lithiated‐graphite for LIBs, but also an effective strategy to develop diverse high‐energy batteries for stationary energy storage in the future. Applications of graphite intercalation compounds as anodes in alkali ion batteries and as cathodes in aluminium‐ion batteries are briefly reviewed in this Progress Report. We also reach conclusions on the drawbacks, major progress, emerging challenges, and some perspectives on the development of graphite intercalation compounds for metal (Li, Na, K, Al) ion batteries.

The use of TiO 2 as an anode in rechargeable sodium-ion batteries (NIBs) is hampered by intrinsic low electronic conductivity of TiO 2 and inferior electrode kinetics. Here, a high-performance TiO 2 electrode for NIBs is presented by designing a multichannel porous TiO 2 nanofibers with well-dispersed Cu nanodots and Cu 2+ -doping derived oxygen vacancies (Cu-MPTO). The in-situ grown well-dispersed copper nanodots of about 3 nm on TiO 2 surface could significantly enhance electronic conductivity of the TiO 2 fibers. The one-dimensional multichannel porous structure could facilitate the electrolyte to soak in, leading to short transport path of Na + through carbon toward the TiO 2 nanoparticle. The Cu 2+ -doping induced oxygen vacancies could decrease the bandgap of TiO 2 , resulting in easy electron trapping. With this strategy, the Cu-MPTO electrodes render an outstanding rate performance for NIBs (120 mAh·g −1 at 20 C) and a superior cycling stability for ultralong cycle life (120 mAh·g −1 at 20 C and 96.5% retention over 2,000 cycles). Density functional theory (DFT) calculations also suggest that Cu 2+ doping can enhance the conductivity and electron transfer of TiO 2 and lower the sodiation energy barrier. This strategy is confirmed to be a general process and could be extended to improve the performance of other materials with low electronic conductivity applied in energy storage systems.

High energy density lithium metal batteries (LMBs) are promising next‐generation energy storage devices. However, the uncontrollable dendrite growth and huge volume change limit their practical applications. Here, a new Mg doped Li–LiB alloy with in situ formed lithiophilic 3D LiB skeleton (hereinafter called Li–B–Mg composite) is presented to suppress Li dendrite and mitigate volume change. The LiB skeleton exhibits superior lithiophilic and conductive characteristics, which contributes to the reduction of the local current density and homogenization of incoming Li+ flux. With the introduction of Mg, the composite achieves an ultralong lithium deposition/dissolution lifespan (500 h, at 0.5 mA cm−2) without short circuit in the symmetrical battery. In addition, the electrochemical performance is superior in full batteries assembled with LiCoO2 cathode and the manufactured composite. The currently proposed 3D Li–B–Mg composite anode may significantly propel the advancement of LMB technology from laboratory research to industrial commercialization. A Li–B–Mg composite with in situ formed 3D LiB fiber network shows a dendrite‐free morphology and less volume change during cycling. The symmetrical battery achieves a long and stable cycle lifespan of more than 500 h at 0.5 mA cm−2 due to the effect of skeleton and the addition of Mg. The full battery also displays improved electrochemical performance.

High‐entropy alloys (HEAs) materials, as promising nanomaterials, have garnered significant attention from researchers due to their excellent performance in the field of hydrogen evolution reaction (HER). The four core effects of HEAs, including the high‐entropy effect, severe lattice distortion effect, sluggish diffusion effect, and cocktail effect, are pivotal in underpinning their remarkable mechanical and thermodynamic properties. Nevertheless, the intricate geometric and electronic structures of HEAs make their catalytic mechanisms exceptionally complex and challenging to decipher. In particular, a thorough analysis of the underlying factors responsible for the outstanding catalytic activity, selectivity, and the ability to maintain stable hydrogen production, even at high current densities, in HEAs is lacking. To provide a systematic exploration of the design and application of HEAs in HER systems, this review commences with an examination of the physicochemical properties of HEAs. It covers a wide range of topics, including the synthesis methods of HEAs, and the major reaction mechanisms of HERs, and presents innovative methods and approaches for designing HEAs specifically in the context of HERs. This paper provides a comprehensive review of the preparation methods for high‐entropy alloys (HEAs) and analyzes their application as catalysts in the hydrogen evolution reaction (HER).

Serious challenges in energy and the environment require us to find solutions that use sustainable processes. There are many sustainable electrocatalytic processes that might provide the answers to the above-mentioned challenges, such as the oxygen reduction reaction (ORR), water splitting, the carbon dioxide reduction reaction (CO 2 RR), and the nitrogen reduction reaction (NRR). These reactions can enhance the value added by producing hydrogen energy through water splitting or convert useless CO 2 and N 2 into fuels and NH 3 . These electrocatalytic reactions can be driven by high-performance catalysts. Therefore, the exploration of novel electrocatalysts is one of the important electrocatalytic fields. In this paper, we aim to systematically discuss a variety of electrocatalysts used for sustainable processes and to give further insights into their status and associated challenges. We invited many famous research groups to write this roadmap with topics including platinum (Pt) and its alloys for ORR, oxides for ORR, chalcogenides for ORR, carbon-based hollow electrocatalysts for ORR, carbides for ORR, atomically dispersed Fe–N–C catalysts for ORR, metal-free catalysts for ORR, single-atom catalysts (SACs) for ORR, metal boride (MB) electrocatalysts for water splitting, transitional metal carbides (TMCs) for water splitting, transition metal (TM) phosphides for water splitting, oxides for water splitting, sulfides for water splitting, layered double hydroxides for water splitting, carbon-based electrocatalysts for water splitting, Ru-based electrocatalysts for water splitting, metal oxides for CO 2 RR, metal sulfides for CO 2 RR, metals for CO 2 RR, carbon for CO 2 RR, SACs for CO 2 RR, heterogeneous molecular catalysts for CO 2 RR, oxides for NRR, chalcogenides for NRR, C 3 N 4 for NRR, SACs for NRR, etc. Their contributions enabled us to compile this 2020 roadmap on electrocatalysts for green catalytic processes and provide some suggestions for future researchers.

Electrochemical nitrogen reduction reaction (eNRR) is one of the most important chemical reactions for the production of ammonia under ambient environment. However, the lack of in-depth understanding of the structure-activity relationship impedes the development of high-performance catalysts for ammonia production. Herein, the density functional theory (DFT) calculations are performed to reveal the structure-activity relationship for the single-atom catalysts (SACs) supported on g-C 3 N 4 , which is modified by molecular groups (i.e., H, O, and OH). The computational results demonstrate that the W-based SACs are beneficial to produce ammonia with a low limiting potential ( U L ). Particularly, the W-OH@g-C 3 N 4 catalyst exhibits an ultralow U L of −0.22 V for eNRR. And the competitive eNRR selectivity can be identified by the dominant *N 2 adsorption free energy than that of *H. Our findings provide a theoretical basis for the synthesis of efficient catalysts to produce ammonia.