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As a typical class of single‐atom catalysts (SACs) possessing prominent advantages of high reactivity, high selectivity, high stability, and maximized atomic utilization, emerging metal‐nitrogen‐doped carbon (M‐N‐C) materials, wherein dispersive metal atoms are coordinated to nitrogen atoms doped in carbon nanomaterials, have presented a high promise to replace the conventional metal or metal oxides‐based catalysts. In this work, recent progress in M‐N‐C‐based materials achieved in both theoretical and experimental investigations is summarized and general principles for novel catalysts design from electronic structure modulating are provided. Firstly, the applications and mechanisms on the advantages and challenges of M‐N‐C‐based materials for a variety of sustainable fuel generation and bioinspired reactions, including the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), hydrogen evolution reaction (HER), carbon dioxide reduction reaction (CO2RR), nitrogen reduction reaction (NRR), and nanozyme reactions are reviewed. Then, strategies toward enhancing the catalytic performance by engineering the nature of metal ion centers, coordinative environment of active centers, carbon support, and their synergistic cooperation, are proposed. Finally, prospects for the rational design of next generation high‐performance M‐N‐C‐based catalysts are outlined. It is expected that this work will provide insights into high‐performance catalysts innovation for sustainable and environmental technologies. The rational design of metal‐nitrogen‐doped carbon (M‐N‐C) materials is at the cutting‐edge of materials research. Herein, the recent progress of M‐N‐C in sustainable fuel generation and biological applications is reviewed. General principles toward designing high‐performance M‐N‐C based nanocatalysts by engineering the nature of metal ion centers, the coordinative environment of active centers, the carbon support, and beyond are outlined.

Water electrolysis is an emerging energy conversion technology, which is significant for efficient hydrogen (H2) production. Based on the high‐activity transition metal ions and metal alloys of ultrastable bifunctional catalyst, the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are the key to achieving the energy conversion method by overall water splitting (OWS). This study reports that the Co‐based coordination polymer (ZIF‐67) anchoring on an indium–organic framework (InOF‐1) composite (InOF‐1@ZIF‐67) is treated followed by carbonization and phosphorization to successfully obtain CoP nanoparticles–embedded carbon nanotubes and nitrogen‐doped carbon materials (CoP‐InNC@CNT). As HER and OER electrocatalysts, it is demonstrated that CoP‐InNC@CNT simultaneously exhibit high HER performance (overpotential of 153 mV in 0.5 m H2SO4 and 159 mV in 1.0 m KOH) and OER performance (overpotential of 270 mV in 1.0 m KOH) activities to reach the current density of 10 mA cm−2. In addition, these CoP‐InNC@CNT rods, as a cathode and an anode, can display an excellent OWS performance with η10 = 1.58 V and better stability, which shows the satisfying electrocatalyst for the OWS compared to control materials. This method ensures the tight and uniform growth of the fast nucleating and stable materials on substrate and can be further applied for practical electrochemical reactions. A type of CoP embedded in carbon nanotubes and nitrogen‐doped carbon material calcined from a bimetallic metal–organic frameworks (MOF) precursor is designed and prepared by growing Co‐based MOFs on an indium–organic framework. The CoP incorporation can greatly promote the water splitting kinetics by the optimized catalyst of CoP‐InNC@CNT, thus the high electrocatalytic activity is achieved toward both the hydrogen evolution reaction and oxygen evolution reaction.

Silicon suboxide (SiOx) has attracted widespread interest as Li‐ion battery (LIB) anodes. However, its undesirable electronic conductivity and apparent volume effect during cycling impede its practical applications. Herein, sustainable rice husks (RHs)‐derived SiO2 are chosen as a feedstock to design SiOx/iron–nitrogen co‐doped carbon (Fe–N–C) materials. Using a facile electrospray‐carbonization strategy, SiOx nanoparticles (NPs) are encapsulated in the nitrogen‐doped carbon (N–C) frameworks decorating atomically dispersed iron sites. Systematic characterizations including high‐angle annular dark‐field scanning transmission electron microscopy (HAADF‐STEM) and X‐ray absorption fine structure (XAFS) verify the existence of Fe single atoms and typical coordination environment. Benefiting from its structural and compositional merits, the SiOx/Fe–N–C anode delivers significantly improved discharge capacity of 799.1 mAh g−1, rate capability, and exceptional durability, compared with pure SiO2 and SiOx/N–C, which has been revealed by the density functional theory (DFT) calculations. Additionally, the electrochemical tests and in situ X‐ray diffraction (XRD) analysis reveal the oxidation of LixSi phase and the storage mechanism. The synthetic strategy is universal for the design and synthesis of metal single atoms/clusters dispersed N–C frameworks encapsulated SiOx NPs. Meanwhile, this work provides impressive insights into developing various LIB anode materials suffering from inferior conductivity and huge volume fluctuations. A universal and facile electrospray‐carbonization strategy is adopted for synthesizing silicon oxide/iron‐nitrogen co‐doped carbon (SiOx/Fe–N–C) materials, which utilizes sustainable rice husks as silicon sources. The Fe–N–C frameworks decorating atomic dispersed Fe sites are employed as the disperse medium of SiOx nanoparticles, facilitating the ion diffusion and charge transfer, accommodating the volume change, and electrochemical reversibility for lithium storage.

This work reports a novel approach for the synthesis of FeCo alloy nanoparticles (NPs) embedded in the N,P‐codoped carbon coated nitrogen‐doped carbon nanotubes (NPC/FeCo@NCNTs). Specifically, the synthesis of NCNT is achieved by the calcination of graphene oxide‐coated polystyrene spheres with Fe3+, Co2+ and melamine adsorbed, during which graphene oxide is transformed into carbon nanotubes and simultaneously nitrogen is doped into the graphitic structure. The NPC/FeCo@NCNT is demonstrated to be an efficient and durable bifunctional catalyst for oxygen evolution (OER) and oxygen reduction reaction (ORR). It only needs an overpotential of 339.5 mV to deliver 10 mA cm−2 for OER and an onset potential of 0.92 V to drive ORR. Its bifunctional catalytic activities outperform those of the composite catalyst Pt/C + RuO2 and most bifunctional catalysts reported. The experimental results and density functional theory calculations have demonstrated that the interplay between FeCo NPs and NCNT and the presence of N,P‐codoped carbon structure play important roles in increasing the catalytic activities of the NPC/FeCo@NCNT. More impressively, the NPC/FeCo@NCNT can be used as the air‐electrode catalyst, improving the performance of rechargeable liquid and flexible all‐solid‐state zinc–air batteries. The FeCo alloy nanoparticles embedded in the N,P‐codoped carbon coated nitrogen‐doped carbon nanotubes (NPC/FeCo@NCNT) have been synthesized and demonstrated to be efficient and durable catalysts for oxygen evolution and reduction reactions. It is usable as the air‐electrode catalysts to improve the performance of rechargeable liquid and flexible all‐solid‐state zinc–air batteries.

Developing high‐performance, low‐cost, and robust bifunctional electrocatalysts for overall water splitting is extremely indispensable and challenging. It is a promising strategy to couple highly active precious metals with transition metals as efficient electrocatalysts, which can not only effectively reduce the cost of the preparation procedure, but also greatly improve the performance of catalysts through a synergistic effect. Herein, Ru and Ni nanoparticles embedded within nitrogen‐doped carbon nanofibers (RuNi‐NCNFs) are synthesized via a simple electrospinning technology with a subsequent carbonization process. The as‐formed RuNi‐NCNFs represent excellent Pt‐like electrocatalytic activity for the hydrogen evolution reaction (HER) in both alkaline and acidic conditions. Furthermore, the RuNi‐NCNFs also exhibit an outstanding oxygen evolution reaction (OER) activity with an overpotential of 290 mV to achieve a current density of 10 mA cm−2 in alkaline electrolyte. Strikingly, owing to both the HER and OER performance, an electrolyzer with RuNi‐NCNFs as both the anode and cathode catalysts requires only a cell voltage of 1.564 V to drive a current density of 10 mA cm−2 in an alkaline medium, which is lower than the benchmark of Pt/C||RuO2 electrodes. This study opens a novel avenue toward the exploration of high efficient but low‐cost electrocatalysts for overall water splitting. A facile strategy based on electrospinning and a postcarbonization process is demonstrated to prepare carbon nanofibers incorporating Ru and Ni nanoparticles, which exhibits admirable Pt‐like hydrogen evolution reaction activity and superior oxygen evolution reaction performance. The electrolyzer with this hybrid as both anode and cathode displays a remarkable electrocatalytic activity and outstanding long‐term durability, which outperforms the commercial Pt/C||RuO2 electrocatalyst.

The rational design of multicomponent heterostructure is an effective strategy to enhance the catalytic activity of electrocatalysts for water and seawater electrolysis in alkaline conditions. Herein, MOF‐derived nitrogen‐doped carbon/nickel‐cobalt sulfides coupled vertically aligned Rhenium disulfide (ReS2) on carbon cloth (NC‐CoNi2S4@ReS2/CC) are constructed via hydrothermal and activation approaches. Experimental and theoretical analysis demonstrates that the strong interactions between multiple interfaces promote electron redistribution and facilitate water dissociation, thereby optimizing *H adsorption energy for the hydrogen evolution reaction (HER). Meanwhile, the adsorption energies of oxygenated intermediates are balanced to reduce the thermodynamic barrier for the oxygen evolution reaction (OER). Consequently, NC‐CoNi2S4@ReS2/CC shows smaller overpotentials of 87 and 253 mV for HER and OER at 10 mA cm−2, with a lower Tafel slope and Rct than control samples. Superior catalytic stability is confirmed by cyclic voltammetry (CV) for 1000 cycles and CA test for 56 h. Furthermore, NC‐CoNi2S4@ReS2/CC presents exceptional electrocatalytic activity in both alkaline water/seawater electrolytes. Stability assessments reveal that NC‐CoNi2S4@ReS2/CC maintains a highly catalytic activity in both water and seawater, owing to the corrosion‐resistant properties of the sulfur species at the interface. These findings highlight the importance of designing heterostructure electrocatalysts for clean hydrogen production. The growth of ReS2 nanosheets on MOF derived metal sulfides catalyst shows excellent catalytic activity for alkaline seawater splitting, attributing to the controllable morphological structure and the rational interfacial design. The heterostructure can inhibit the restacking of ReS2 nanosheets to expose abundant edge active sites, facilitate electron transfer and boost the active sites to improve the electrocatalytic performance.

At present, it is still a challenge to prepare multifunctional composite nanomaterials with simple composition and favorable structure. Here, multifunctional Fe3O4@nitrogen-doped carbon (N-C) nanocomposites with hollow porous core-shell structure and significant electrochemical, adsorption and sensing performances were successfully synthesized through the hydrothermal method, polymer coating, then thermal annealing process in nitrogen (N2) and lastly etching in hydrochloric acid (HCl). The morphologies and properties of the as-obtained Fe3O4@N-C nanocomposites were markedly affected by the etching time of HCl. When the Fe3O4@N-C nanocomposites after etching for 30 min (Fe3O4@N-C-3) were applied as the anodes for lithium-ion batteries (LIBs), the invertible capacity could reach 1772 mA h g−1 after 100 cycles at the current density of 0.2 A g−1, which is much better than that of Fe3O4@N-C nanocomposites etched, respectively, for 15 min and 45 min (948 mA h g−1 and 1127 mA h g−1). Additionally, the hollow porous Fe3O4@N-C-3 nanocomposites also exhibited superior rate capacity (950 mA h g−1 at 0.6 A g−1). The excellent electrochemical properties of Fe3O4@N-C nanocomposites are attributed to their distinctive hollow porous core-shell structure and appropriate N-doped carbon coating, which could provide high-efficiency transmission channels for ions/electrons, improve the structural stability and accommodate the volume variation in the repeated Li insertion/extraction procedure. In addition, the Fe3O4@N-C nanocomposites etched by HCl for different lengths of time, especially Fe3O4@N-C-3 nanocomposites, also show good performance as adsorbents for the removal of the organic dye (methyl orange, MO) and surface-enhanced Raman scattering (SERS) substrates for the determination of a pesticide (thiram). This work provides reference for the design and preparation of multifunctional materials with peculiar pore structure and uncomplicated composition.

Dual‐ion batteries (DIBs) are often criticized for their low discharge capacity and poor cyclic capability despite their inherent high working voltage, low manufacturing cost, and environmental friendliness. To solve these shortcomings, many attempts and efforts have been devoted, but all ended in unsatisfactory results. Herein, a hierarchical porous carbon nanosphere anode with ultrahigh nitrogen doping is developed, which exhibits fast ion transport kinetics and excellent Li+ storage capability. Moreover, employing a concentrated electrolyte is expected to bring a series of advantages such as stable SEI for facilitating ion transmission, enhanced cycling performance, high specific capacity, and operation voltage. These advantages endow the assembled full DIBs with excellent performance as a super‐high specific discharge capacity of 351 mAh g−1 and can be cycled stably for 1300 cycles with Coulombic efficiency (CE) remaining at 99.5%; a high operating voltage range of 4.95–3.63 V and low self‐discharge rate of 2.46% h−1 with stable fast charging‐slow discharging performance. Through electrochemical measurements and physical characterizations, the possible working mechanism of the proof‐of‐concept full battery and the structural variations of electrodes during cycling are investigated. The design strategy of novel battery system in this work will promote the development of high‐performance DIBs. The working mechanism of the proof‐of‐concept full battery.

Precious metal‐based single‐atom catalysts (PM‐SACs) hosted in N‐doped carbon supports have shown new opportunities to revolutionize cathodic oxygen reduction reaction (ORR). However, stabilizing the high density of PM‐Nx sites remains a challenge, primarily due to the inherently high free energy of isolated metal atoms, predisposing them to facile atomic agglomeration. Herein, a molten salt‐assisted synthesis strategy is proposed to prepare porous PM1/N‐CPores (PM = Ru, Pt, and Pd) electrocatalysts with densely accessible PM‐Nx sites. A hierarchically porous N‐doped carbon substrate (N‐CPores), synthesized via the NaCl‐assisted pyrolysis of zeolitic imidazolate framework‐8, effectively improves the utilization of PM‐Nx sites by increased reactants accessible surface area and reduced mass transfer resistance. In accordance with theoretical calculations, the as‐prepared Ru1/N‐CPores, featuring superior intrinsic active Ru‐N4 sites, exhibit outstanding ORR turnover frequency of 6.19 e− site−1 s−1, and outperforms the commercial Pt/C with a 5.3‐fold of mass activity (5.83 ± 0.61 A mg−1) at 0.8 V versus reversible hydrogen electrode. The commendable activity and stability of Ru1/N‐CPores in a real fuel cell device further affirm its practical applicability. A series of porous precious metal‐based single‐atom electrocatalysts (PM1/N‐CPores, PM = Ru, and Pt, Pd), fabricated by molten salt‐assisted pyrolysis strategy, achieved a high density of catalytically accessible PM single‐atom sites. Owing to the hierarchical porous structure and the abundant highly active Ru single‐atom sites, the as‐prepared Ru1/N‐CPores exhibit significantly promoted oxygen reduction reaction (ORR) activity in acid electrolytes.

Interfacial solar evaporation, which captures solar energy and localizes the absorbed heat for water evaporation, is considered a promising technology for seawater desalination and solar energy conversion. However, it is currently limited by its low photothermal conversion efficiency, salt accumulation, and poor reliability. Herein, inspired by human intestinal villi structure, we design and fabricate a novel intestinal villi‐like nitrogen‐doped carbon nanotubes solar steam generator (N‐CNTs SSG) consisting of three‐dimensional (3D) hierarchical carbon nanotube matrices for ultrahigh solar evaporation efficiency. The 3D matrices with radial direction nitrogen‐doped carbon nanotube clusters achieve ultrahigh surface area, photothermal efficiency, and hydrophilicity, which significantly intensifies the whole interfacial solar evaporation process. The new solar evaporation efficiency reaches as high as 96.8%. Furthermore, our ab initio molecular dynamics simulation reveals that N‐doped carbon nanotubes exhibit a greater number of electronic states in close proximity to the Fermi level when compared to pristine carbon nanotubes. The outstanding absorptivity in the full solar spectrum and high solar altitude angles of the 3D hierarchical carbon nanotube matrices offer great potential to enable ultrahigh photothermal conversion under all‐day and all‐season circumstances. Inspired by the intestinal villi structure and quasi‐blackbody feature of nitrogen‐doped carbon nanotubes, a novel intestinal villi‐like nitrogen‐doped carbon nanotubes solar steam generator (N‐CNTs SSG) was designed and fabricated. Benefitting from the multi‐reflection and diffuse reflection, the novel N‐CNTs SSG achieves multi‐angle all‐weather sunlight absorption and unprecedentedly high solar evaporation efficiency of 96.8%.