In recent years, investigations into atomic catalysts has accelerated significantly. Although different atomic catalysts have been developed, the introduction of main group elements is rarely considered. In this work, the possibility of introducing alkaline/alkaline earth metals (AAEM), post‐transition metal (Post‐TM), and metalloids to form stable graphdiyne‐based dual atomic catalysts (GDY‐DAC) is revealed. The main group elements not only act as a promising separator to improve the loading of DACs but also activate the alkyl chains to facilitate the electroactivity of GDY‐DAC. Most importantly, the main group elements in the GDY‐DAC do not affect the electroactivity of transition or lanthanide metals and even enable subtle modulations on the electronic structures. The p band center is a significant descriptor to modulate the electroactivity in oxides while their applications in the atomic catalysts are unclear. With the further evaluations of machine learning, it is found that the involvements of s‐orbitals and p‐orbitals perturb the prediction accuracies of both formation energies and p‐band center, especially for the AAEM. This work supplies insights that are expected to aid progress in designing main group elements‐based atomic catalysts, which opens a new avenue in designing advanced electrocatalysts.

Rare earth (RE) based halide solid electrolytes (HEs) are recently considered as research hotspots in the field of all‐solid‐state batteries (ASSBs). The RE‐based HEs possess high ionic conductivity, credible deformability, and good stability, which can bring excellent electrochemical performances for ASSBs. However, the conventional synthetic methods of RE HEs are a mechanochemical process and co‐melting strategy, both approaches require expensive raw materials and sophisticated equipment. Therefore, a lot of research work is required to promote the preparation methods for these promising SSEs in ASSBs. Thus, a vacuum evaporation‐assisted synthesis method is developed for the massive synthesis of HEs. The as‐prepared Li3HoBr6 (LHB) has a high lithium‐ion conductivity close to the mS cm−1 level and the LHB‐based Li‐Se ASSBs can be assembled by cold pressing. Theoretical calculations have revealed that the Li migrations are highly preferred in Li3HoBr6 owing to the low energy cost and high tolerance of stable structure. The tetrahedral and octahedral pathways are responsible for Li migrations in short and long ranges, respectively. The results show that the LHB‐based Li‐Se battery has good stability and rate performance, indicating that LHB has potential application in the field of ASSBs.

Electroreduction of CO2 has become the most attractive approach to generate value‐added chemicals and fuels. Products of single atomic catalysts (SAC) in CO2 reduction reaction reactions (CO2RR) are mostly limited to CO since the contributions of spatial and thermodynamic factors are not distinguished. To break through the challenges, comprehensive explorations in graphdiyne(GDY)‐based SAC are made, to reveal detailed influences of active sites, elements, and adsorptions on the selectivity and reaction energy of the C1 pathway. Unique d electrons dominated adsorption behaviors are identified, where the d6 boundary is able to help screen out promising candidates for achieving complicated C2+ products. Based on spatial and thermodynamic factors, metal sites are still the most promising active sites. The transition metal based GDY‐SACs show element‐dependent electroactivity towards different products in CO2RR. Meanwhile, the GDY‐Pr and GDY‐Pm SACs are promising candidates for the CO2RR and even C2 products in the future. This work supplies in‐depth insights into the CO2RR to facilitate the design of efficient atomic catalysts in future work.

fossil fuels, which account for 70% of the greenhouse gases in the atmosphere and have a profound impact on the global warming issue. Carbon neutrality is critical to address the climate crisis, which requires immediate actions from the global community. China has also set the development goal of reaching the carbon emission peak in 2030 and carbon neutrality in 2060. In recent years, there has been increasing attention and efforts in the technology advances for zero or even negative emissions to accelerate the developments toward carbon neutrality. In particular, carbon capture, utilization, and storage (CCUS) technology are one of the important methods to effectively reduce carbon emissions. As a potential carbon resource compound, carbon dioxide (CO 2 ) can be converted into high-value-added chemicals, carbon-based fuels, and other small molecules with broad applications in industries, which supplies practical solutions for the greenhouse effect. Especially, electrochemical CO 2 reduction reaction (CO 2 RR) represents one of the most promising approaches to capturing and utilizing CO 2 from the atmosphere. [1][2][3] Depending on the electrocatalysts, CO 2 RR can be accomplished via different pathways that involve varied electrons and products from the C 1 products (e.g., CO, HCOOH, and CH 4 ) to valuable C 2 products (e.g., C 2 H 4 , CH 3 CH 2 OH, CH 3 CHO, CH 3 COOH, etc.) for broad applications. [4][5][6][7] Compared to widely reported C 1 products, the generation of complicated C 2 products is still highly challenging with several key bottlenecks to be overcome including large overpotential and low selectivity and faradaic efficiency (FE) of target products, which are attributed to the complicated reaction mechanism with multi-electron transfer processes. [8] Currently, many different electrocatalysts have been reported for CO 2 RR including noble metals and alloys (e.g., Pd, Ag, Au, and Cu), oxides (e.g., Cu x O, SnO 2 , etc.), as well as composite electrocatalysts. [3,[9][10][11][12] However, the generation of valuable multi-carbon products (C 2 and C 2+ products) still mostly depends on the Cu-based electrocatalysts. [3,[13][14][15][16] Recently, the fast developments of atomic catalysts (ACs) have been widely reported in many different energy and Developing efficient and stable atomic catalysts (ACs) to achieve high faradaic efficiency and selectivity of C 2 products is a significant challenge for research on the CO 2 reduction reaction (CO 2 RR). Although significant efforts have been devoted to this endeavor, the understanding of C 2 pathways and the influences of metal selection and active sites on the CO 2 RR still remain unclear. Herein, this work presents a comprehensive theoretical exploration of full C 2 reaction pathway mapping based on graphdiyne (GDY)-supported ACs with considerations of different metals and active sites for the first time. This work demonstrates the integrated large-small cycle mechanism to explain the challenges for C 2 product generation, where the double-dependence correl...

The urgent demand for sustainable energy resources has boosted the research of highly efficient electrocatalysts for the hydrogen evolution reaction (HER). However, the majority of the reported catalysts have been...