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Enabling high‐efficiency solar thermal conversion (STC) at catalytic active site is critical but challenging for harnessing solar energy to boost catalytic reactions. Herein, we report the direct integration of full‐spectrum STC and high electrocatalytic oxygen evolution activity by fabricating a hierarchical nanocage architecture composed of graphene‐encapsulated CoNi nanoparticle. This catalyst exhibits a near‐complete 98 % absorptivity of solar spectrum and a high STC efficiency of 97 %, which is superior than previous solar thermal catalytic materials. It delivers a remarkable potential decrease of over 240 mV at various current densities for electrocatalytic oxygen evolution under solar illumination, which is practically unachievable via traditionally heating the system. The high‐efficiency STC is enabled by a synergy between the regulated electronic structure of graphene via CoNi‐carbon interaction and the multiple absorption of lights by the light‐trapping nanocage. Theoretical calculations suggest that high temperature‐induced vibrational free energy gain promotes the potential‐limiting *O to *OOH step, which decreases the overpotential for oxygen evolution. [ABSTRACT FROM AUTHOR]

The electrocatalytic synthesis of C–N coupling compounds from CO2 and nitrogenous species not only offers an effective avenue to achieve carbon neutrality and reduce environmental pollution, but also establishes a route to synthesize valuable chemicals, such as urea, amide, and amine. This innovative approach expands the application range and product categories beyond simple carbonaceous species in electrocatalytic CO2 reduction, which is becoming a rapidly advancing field. This review summarizes the research progress in electrocatalytic urea synthesis, using N2, NO2−, and NO3− as nitrogenous species, and explores emerging trends in the electrosynthesis of amide and amine from CO2 and nitrogen species. Additionally, the future opportunities in this field are highlighted, including electrosynthesis of amino acids and other compounds containing C–N bonds, anodic C–N coupling reactions beyond water oxidation, and the catalytic mechanism of corresponding reactions. This critical review also captures the insights aimed at accelerating the development of electrochemical C–N coupling reactions, confirming the superiority of this electrochemical method over the traditional techniques. [ABSTRACT FROM AUTHOR]

The article in the journal "Angewandte Chemie International Edition" discusses the development of a solar thermal electrocatalyst that enhances oxygen evolution through full-spectrum light-harvesting. Researchers, including Dehui Deng and Liang Yu, have created a hierarchical nanocage architecture that achieves high solar absorptivity and lowers the potential for the oxygen evolution reaction. This innovative approach could significantly improve the efficiency of catalytic reactions powered by solar energy. [Extracted from the article]

The article in Angewandte Chemie discusses the development of a highly efficient solar thermal conversion (STC) catalyst for boosting catalytic reactions using solar energy. Researchers, including Dehui Deng and Liang Yu, integrated full-spectrum STC and electrocatalytic oxygen evolution activity on a "Chainmail" catalyst with a hierarchical nanocage architecture. This innovation achieved a 98% solar absorptivity and significantly decreased the potential for the oxygen evolution reaction by over 240 mV. [Extracted from the article]

Developing stable but high active metal-nitrogen-carbon (M-N-C)-based hard carbon anode is a promising way to be the alternatives to graphene and blank hard carbon for sodium-ion batteries (SIBs), requiring the precise tailoring of the electronic structure for optimizing the Na+ intercalation behavior, yet is greatly challenging. Herein, Fe-N-C graphitic layer-encapsulating Fe3C species within hard carbon nanosheets (Fe-N-C/Fe3C@HCNs) are rationally engineered by pyrolysis of self-assembled polymer. Impressively, the Fe-N-C/Fe3C@HCNs exhibit outstanding rate capacity (242 mAh·g−1 at 2,000 mA·g−1), which is 2.1 and 4.2 times higher than that of Fe-N-C and N-doped carbon (N-C), respectively, and prolonged cycling stability (176 mAh·g−1 at 2,000 mA·g−1 after 2,000 cycles). Theoretical calculations unveil that the Fe3C species enhance the electronic transfer from Na to Fe-N-C, resulting in the charge redistribution between the interfaces of Fe3C and Fe-N-C. Thus, the optimized adsorption behavior towards Na+ reduces the thermodynamic energy barriers. The synergistic effect of Fe3C and Fe-N-C species maintains the structural integrity of electrode materials during the sodiation/desodiation process. The in-depth insight into the advanced Na+ storage mechanisms of Fe3C@Fe-N-C offers precise guidance for the rational establishment of confinement heterostructures in SIBs. [ABSTRACT FROM AUTHOR]

Layered transition-metal oxyhydroxides (MOOHs) emerge as promising noble-metal-free electrocatalysts for the oxygen evolution reaction (OER), yet are subject to a limited number of active sites at edges with an inactive basal plane. Herein, we report that a large number of in-plane active sites can be generated by confining high density of 16 wt% molybdenum single atoms in the basal-plane lattice of CoOOH (Mo-CoOOH). By constructing robust three-dimensional (3D) nanoframes to prevent layer-stacking and maximize exposure of active basal planes, the catalyst achieves an unprecedented OER activity at a large current density of 2000 mA cm−2, exhibiting the lowest overpotential of 400 mV among all previously reported catalysts with a high durability of over 120 hours. Multiple spectrometry characterization studies and first-principles calculations reveal that lattice-confined Mo atoms can bond moderately with OER intermediates, thereby serving as active sites for the reaction. This strategy provides a new path to design high-performance MOOH electrocatalysts with rich in-plane active sites. [ABSTRACT FROM AUTHOR]

Perturbing the electronic structure of the MoS2 basal plane by confining heteroatoms offers the opportunity to trigger in‐plane activity for the hydrogen evolution reaction (HER). The key challenge consists of inducing the optimum HER activity by controlling the type and distribution of confined atoms. A distance synergy of MoS2‐confined single‐atom rhodium is presented, leading to an ultra‐high HER activity at the in‐plane S sites adjacent to the rhodium. By optimizing the distance between the confined Rh atoms, an ultra‐low overpotential of 67 mV is achieved at a current density of 10 mA cm−2 in acidic solution. Experiments and first‐principles calculations demonstrate a unique distance synergy between the confined rhodium atoms in tuning the reactivity of neighboring in‐plane S atoms, which presents a volcanic trend with the inter‐rhodium distance. This study provides a new strategy to tailor the activity of MoS2 surface via modulating the distance between confined single atoms. [ABSTRACT FROM AUTHOR]

Electrocatalytic CO2 reduction to CO is a sustainable process for energy conversion. However, this process is still hindered by the diffusion-limited mass transfer, low electrical conductivity and catalytic activity. Therefore, new strategies for catalyst design should be adopted to solve these problems and improve the electrocatalytic performance for CO production. Herein, we report a multiscale carbon foam confining single iron atoms prepared with the assistant of SiO2 template. The pore-enriched environment at the macro-scale facilitates the diffusion of reactants and products. The graphene nanosheets at the nano-scale promote the charge transfer during the reaction. The single iron atoms confined in carbon matrix at the atomic-scale provide the active sites for electrocatalytic CO2 reduction to CO. The optimized catalyst achieves a CO Faradaic efficiency of 94.9% at a moderate potential of −0.5 V vs. RHE. Furthermore, the performance can be maintained over 60 hours due to the stable single iron atoms coordinated with four nitrogen atoms in the carbon matrix. This work provides a promising strategy to improve both the activity and stability of single atom catalysts for electrocatalytic CO2 reduction to CO. [ABSTRACT FROM AUTHOR]

Tin-based materials have been designed as potential catalysts for the electrochemical conversion of CO 2 into a single product. However, such tin-based materials still face the challenges of unsatisfactory selectivity, because the rate-determining step is situated within the slow desorption step. In this work, a variety of tin-based materials are synthesized using the electrospinning technique in an effort to control the adsorption strength during electrochemical reduction, therefore improving the selectivity of CO 2 reduction toward formate. The optimized SnS material exhibits moderate adsorption strength to *OCHO and *HCOOH, and the appropriate atomic distance of Sn-Sn maintained the balanced adsorption posture of both intermediate. Therefore, the rate-determining step can be shifted from the slow desorption of the *HCOOH step (Sn) to the first hydrogenation of the *OCHO species step (SnS). Due to this shift, the SnS/C electrode demonstrated excellent selectivity, with a Faradaic efficiency of 96% for the production of formate. A maximum current density of -12.5 mA cm -2 for formate is also achieved for a period of 33 h., (© 2024 Wiley‐VCH GmbH.)