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To explore the application of neural network algorithm model in lung cancer imaging, and provide reference for the application and development of artificial neural network (ANN) algorithm model in lung cancer medical mirroring, so as to promote the development of ANN in this field. Meanwhile, it is hoped that the application of neural network algorithms in medical imaging can improve the survival rate and cure rate of lung cancer. In this study, an ANN algorithm model was selected to establish a lung cancer recognition model. After determining the lung cancer lesion area, the image segmentation algorithm was used to separately display the lung cancer lesion area, and a comparison experiment was designed to verify the accuracy of the model. ANNs were used to identify lung cancer, which can be concluded that the accuracy is 94.6%, the sensitivity is 95.7%, and the specificity is 93.5%. By combining image retrieval methods with lung cancer image segmentation algorithms, the lesion area of lung cancer can be clearly displayed. Therefore, the lung cancer image segmentation algorithm based on the neural network model has good recognition performance. This research can provide reference for the application of neural network algorithm model in the field of cancer diagnosis and treatment. [ABSTRACT FROM AUTHOR]

Lithium‐metal anodes with excellent theoretical specific capacities (3680 mAh g−1) have attracted considerable attention for overcoming the capacity bottleneck of conventional graphite anodes. However, they often suffer from uncontrolled dendrite growth and undesirable side reactions, considerably limiting their practical application in lithium‐metal batteries. In this study, urchin‐like silver@copper oxide (Ag@CuO) heterostructures with gradient electrical conductivity and lithiophilicity are prepared using a facile liquid‐phase reduction method. The unique amphiphilic lithium mechanism of the alloying and conversion reactions effectively reduces the nucleation overpotential of the lithium metal anode and promotes a uniform lithium deposition process. Meanwhile, the in situ‐generated Li2O‐rich solid electrolyte interphase (SEI) film can further induce uniform and reversible lithium plating/stripping. All these characteristics endow the Ag@CuO anode with a high Coulombic efficiency of 98.89%, even after 1200 cycles, and long cycle life of 2800 h at a current density of 0.2 mA cm−2, thus demonstrating that such modified Li metal anodes exhibit superior compatibility with major commercial cathode materials, such as LiCoO2 (LCO) and LiNi0.8Co0.1Mn0.1O2 (NCM‐811). Hence, this study provides an effective strategy for developing practical lithium metal anodes. [ABSTRACT FROM AUTHOR]

Emerging high entropy compounds (HECs) have attracted huge attention in electrochemical energy‐related applications. The features of ultrafine size and carbon incorporation show great potential to boost the ion‐storage kinetics of HECs. However, they are rarely reported because high‐temperature calcination tends to result in larger crystallites, phase separation, and carbon reduction. Herein, using the NaCl self‐assembly template method, by introducing a high‐pressure field in the calcination process, the atom diffusion and phase separation are inhibited for the general formation of HECs, and the HEC aggregation is inhibited for obtaining ultrafine size. The general preparation of ultrafine‐sized (<10 nm) HECs (nitrides, oxides, sulfides, and phosphates) anchored on porous carbon composites is realized. They are demonstrated by combining advanced characterization technologies with theoretical computations. Ultrafine‐sized high entropy sulfides‐MnFeCoCuSnMo/porous carbon (HES‐MnFeCoCuSnMo/PC) as representative anodes exhibit excellent sodium‐ion storage kinetics and capacities (a high rating capacity of 278 mAh g−1 at 10 A g−1 for full cell and a high cycling capacity of 281 mAh g−1 at 20 A g−1 after 6000 cycles for half cell) due to the combining advantages of high entropy effect, ultrafine size, and PC incorporation. Our work provides a new opportunity for designing and fabricating ultrafine‐sized HECs. [ABSTRACT FROM AUTHOR]

Emerging high entropy compounds (HECs) have attracted huge attention in electrochemical energy‐related applications. The features of ultrafine size and carbon incorporation show great potential to boost the ion‐storage kinetics of HECs. However, they are rarely reported because high‐temperature calcination tends to result in larger crystallites, phase separation, and carbon reduction. Herein, using the NaCl self‐assembly template method, by introducing a high‐pressure field in the calcination process, the atom diffusion and phase separation are inhibited for the general formation of HECs, and the HEC aggregation is inhibited for obtaining ultrafine size. The general preparation of ultrafine‐sized (<10 nm) HECs (nitrides, oxides, sulfides, and phosphates) anchored on porous carbon composites is realized. They are demonstrated by combining advanced characterization technologies with theoretical computations. Ultrafine‐sized high entropy sulfides‐MnFeCoCuSnMo/porous carbon (HES‐MnFeCoCuSnMo/PC) as representative anodes exhibit excellent sodium‐ion storage kinetics and capacities (a high rating capacity of 278 mAh g−1 at 10 A g−1 for full cell and a high cycling capacity of 281 mAh g−1 at 20 A g−1 after 6000 cycles for half cell) due to the combining advantages of high entropy effect, ultrafine size, and PC incorporation. Our work provides a new opportunity for designing and fabricating ultrafine‐sized HECs. [ABSTRACT FROM AUTHOR]

Aluminum‐air battery (AAB) with alkaline‐based aqueous electrolyte have attracted intensive research interests due to high‐capacity density, low cost, and high safety. However, severe hydrogen evolution reaction (HER) of Al anode in alkaline electrolyte extremely restricts its large‐scale application. In this work, ZnO with a group of quaternary ammonium salts (QAS, denoted as C1, C2, C4, C6, and C8 depending on the length of non‐polar group) are introduced into electrolytes to inhibit HER. It is revealing that capacity density initially increases with C1, C2, or C4, up to 2564 mAh gAl−1 with anodic utilization rate of 86.0%, and then follows by a decline (C6 and C8). The addition of QAS creates "physical‐hydrophobic interface" by non‐polar group owing to its electrophilic property and constructs "chemical‐hydrophobic interface" with polar group by reducing water activity. QAS also promotes the uniform growth of Zn‐based film, as a barrier against H2O. Thus, HER is effectively inhibited to improve the capacity density. With further increasing non‐polar group length (C6 or C8), the bonding status of the film deteriorates with enhanced H2O activity, leading to the recurrence of HER. This work explores the effect of non‐polar groups on inhibiting HER and opens the door to stable anodes for alkaline‐based batteries. [ABSTRACT FROM AUTHOR]

The Na3V2(PO4)2F3 (NVPF) cathode material is usually nano‐sized particles exhibiting low tap density, high specific surface area, correspondingly low volume energy density, and cycle stability of the sodium‐ion batteries (SIBs). Herein, a high‐temperature shock (HTS) strategy is proposed to synthesize NVPF (HTS‐NVPF) with uniform conducting network and high tap density. During a typical HTS process (heating rate of 1100 °C s−1 for 10 s), the precursors rapidly crystallize and form large‐sized and dense particles. The tight connection between particles not only enhances their contact with carbon layers, but also reduces the specific surface area that inhibits side reactions between the interfaces and the electrolyte. Besides, ultrafast synthesis of NVPF reduces the F loss and amount of Na3V2(PO4)3 impurities, which improve cycling capability. The HTS‐NVPF demonstrates a high energy density of 413.4 Wh kg−1 and an ultra‐high specific capacity of 103.4 mAh g−1 at 10 C as well as 84.2% capacity retention after 1000 cycles. In addition, the excellent temperature adaptability of HTS‐NVPF (−45–55 °C) and remarkable electrochemical properties of NVPF||HC full cell demonstrate extreme competitiveness in commercial SIBs. Therefore, the HTS technique is considered to be a high‐efficiency strategy to synthetize NVPF and is expected to prepare other cathode materials. [ABSTRACT FROM AUTHOR]

Carbon dioxide electroreduction reaction (CO2RR) can take full advantage of sustainable power to reduce the continuously increasing carbon emissions. Recycling CO2 to produce formic acid or formate is a technologically and economically viable route to accomplish CO2 cyclic utilization. Developing efficient and cost‐effective electrocatalysts with high selectivity towards formate is prioritized for the industrialized applications of CO2RR electrolysis. From the previous explored CO2RR catalysts, Sn, Bi and In based materials have drawn increasing attentions due to the high selectivity towards formate. However, there are still confronted with several challenges for the practical applications of these materials. Therefore, a rational design of the catalysts for formate is urgently needed for the target of industrialized applications. Herein, we comprehensively summarized the recent development in the advanced electrocatalysts for the CO2RR to formate. Firstly, the reaction mechanism of CO2RR is introduced. Then the preparation and design strategies of the highly active electrocatalysts are presented. Especially the innovative design mechanism in engineering materials for promoting catalytic performance, and the efforts on mechanistic exploration using in situ (ex situ) characterization techniques are reviewed. Subsequently, some perspectives and expectations are proposed about current challenges and future potentials in CO2RR research. [ABSTRACT FROM AUTHOR]

Dendrites and side reactions of Zn anodes severely restrict the application of aqueous Zn‐based batteries for grid‐scale energy storage. While surface/interface modification strategies have shown some progress in improving Zn anode reversibility, they still fall short in addressing the overall regulation and intrinsic mechanisms from the bulk‐phase perspective. Herein, a bulk‐phase composite Zn/CNTs anodes fabricated by a powder‐metallurgy‐based strategy is introduced. Benefiting from the regulation of grain boundary engineering on local electric conductivity, electric field distributions, and Zn atom absorption energy, the Zn/CNTs anodes effectively suppress dendrite growth and enhance corrosion resistance during Zn stripping/plating cycles. Symmetrical cells equipped with Zn/CNT4 anodes exhibit extended cycling stability with minimal voltage hysteresis (only 22 mV). Furthermore, the full cells incorporating Zn/CNT4 with commercial MnO2 demonstrate superior rate performance and specific capacitance retention after 500 h cycling. This breakthrough opens up new avenues for optimizing metallic anodes at the bulk phase level using powder metallurgy, enabling scalable manufacturing processes, and providing valuable insights for various metal anode systems. [ABSTRACT FROM AUTHOR]

Aqueous Zn‐based batteries have emerged as compelling candidates for grid‐scale energy storage, owing to their intrinsic safety, remarkable theoretical energy density and cost‐effectiveness. Nonetheless, the dendrite formation, side reactions, and corrosion on anode have overshadowed their practical applications. Herein, we present an in situ grown carbon network reinforcing Zn matrix anode prepared by powder metallurgy. This carbon network provides an uninterrupted internal electron transport pathway and optimize the surface electric field distribution, thereby enabling highly reversible Zn deposition. Consequently, symmetrical cells demonstrate impressive stability, running for over 880 h with a low voltage hysteresis (≈32 mV). Furthermore, this Zn matrix composite anode exhibits enhanced performance in both the aqueous Zn‐ion and the Zn‐air batteries. Notably, Zn//MnO2 cells display superior rate capabilities, while Zn‐air batteries deliver high power density and impressive Zn utilization rate (84.9 %). This work provides a new idea of powder metallurgy method for modified Zn anodes, showcasing potential for large‐scale production. [ABSTRACT FROM AUTHOR]

Aqueous Zn‐based batteries have emerged as compelling candidates for grid‐scale energy storage, owing to their intrinsic safety, remarkable theoretical energy density and cost‐effectiveness. Nonetheless, the dendrite formation, side reactions, and corrosion on anode have overshadowed their practical applications. Herein, we present an in situ grown carbon network reinforcing Zn matrix anode prepared by powder metallurgy. This carbon network provides an uninterrupted internal electron transport pathway and optimize the surface electric field distribution, thereby enabling highly reversible Zn deposition. Consequently, symmetrical cells demonstrate impressive stability, running for over 880 h with a low voltage hysteresis (≈32 mV). Furthermore, this Zn matrix composite anode exhibits enhanced performance in both the aqueous Zn‐ion and the Zn‐air batteries. Notably, Zn//MnO2 cells display superior rate capabilities, while Zn‐air batteries deliver high power density and impressive Zn utilization rate (84.9 %). This work provides a new idea of powder metallurgy method for modified Zn anodes, showcasing potential for large‐scale production. [ABSTRACT FROM AUTHOR]

The catalyst‐reconstruction makes it challenging to clarify the practical active sites and unveil the actual reaction mechanism during the CO2 electroreduction reaction (CO2RR). However, currently the impact of the electrolyte microenvironment in which the electrolyte is in contact with the catalyst is overlooked and might induce a chemical evolution, thus confusing the reconstruction process and mechanism. In this work, the carbonate adsorption properties of metal oxides were investigated, and the mechanism of how the electrolyte carbonate affect the chemical evolution of catalysts were discussed. Notably, Bi2O3 with weak carbonate adsorption underwent a chemical reconstruction to form the Bi2O2CO3/Bi2O3 heterostructure. Furthermore, in situ and ex situ characterizations unveiled the formation mechanism of the heterostructure. The in situ formed Bi2O2CO3/Bi2O3 heterostructure with strong electron interaction served as the highly active structure for CO2RR, achieving a formate Faradaic efficiency of 98.1 % at −0.8 Vvs RHE. Theoretical calculations demonstrate that the significantly tuned p‐orbit electrons of the Bi sites in Bi2O2CO3/Bi2O3 optimized the adsorption of the intermediate and lowered the energy barrier for the formation of *OCHO. This work elucidates the mechanism of electrolyte microenvironment for affecting catalyst reconstruction, which contributes to the understanding of reconstruction process and clarification of the actual catalytic structure. [ABSTRACT FROM AUTHOR]

The catalyst‐reconstruction makes it challenging to clarify the practical active sites and unveil the actual reaction mechanism during the CO2 electroreduction reaction (CO2RR). However, currently the impact of the electrolyte microenvironment in which the electrolyte is in contact with the catalyst is overlooked and might induce a chemical evolution, thus confusing the reconstruction process and mechanism. In this work, the carbonate adsorption properties of metal oxides were investigated, and the mechanism of how the electrolyte carbonate affect the chemical evolution of catalysts were discussed. Notably, Bi2O3 with weak carbonate adsorption underwent a chemical reconstruction to form the Bi2O2CO3/Bi2O3 heterostructure. Furthermore, in situ and ex situ characterizations unveiled the formation mechanism of the heterostructure. The in situ formed Bi2O2CO3/Bi2O3 heterostructure with strong electron interaction served as the highly active structure for CO2RR, achieving a formate Faradaic efficiency of 98.1 % at −0.8 Vvs RHE. Theoretical calculations demonstrate that the significantly tuned p‐orbit electrons of the Bi sites in Bi2O2CO3/Bi2O3 optimized the adsorption of the intermediate and lowered the energy barrier for the formation of *OCHO. This work elucidates the mechanism of electrolyte microenvironment for affecting catalyst reconstruction, which contributes to the understanding of reconstruction process and clarification of the actual catalytic structure. [ABSTRACT FROM AUTHOR]

Defect engineering is demonstrated to be an important factor in enhancing the electrochemical performance of lithium‐ion batteries by improving structural stability and ion diffusion. However, conventional synthetic methods have long and complicated processes, making it challenging to effectively and easily introduce defects into electrode materials. In this work, a high‐temperature shock technique (HTS) with an ultrafast heating and cooling process that can quickly introduce twin boundaries (TBs) into phase‐pure spinel LiMn2O4 in seconds is reported. Various ex situ techniques reveal the crystallization mechanism of LiMn2O4 during ultrafast synthesis. LiMn2O4 with TBs exhibits a higher rate performance than that obtained from the traditional method. Additionally, alien elements can be evenly incorporated into LiMn2O4 in seconds, resulting in excellent cycling performance. For instance, 2% Ni‐doped LiMn2O4 shows an initial capacity of 121 mAh g−1 and retention of 86.5% after 500 cycles at 1 C. [ABSTRACT FROM AUTHOR]

Developing high‐performance anode current collectors with three‐dimensional structure and lithiophilic layers is of great importance to further advance the application of lithium metal batteries. However, relatively few research has focused on the transition of substrate and the intrinsic structure stability after electrodeposition of lithium on substrates, which leads to an incomplete understanding of the behavior of lithium deposition. Herein, a lithium metal anodes host with a highly stable and 3D structure has been effectively produced through in situ development of nanoflake arrays embedded with Co3O4 obtained from ZIF on nickel foams (Co3O4‐NF). And the actual lithium deposition sites and lithium deposition process on Co3O4‐NF are elucidated via a combination of characterization techniques and electrochemical analytical methods. Consequently, the resulting Co3O4‐NF@Li anodes could effectively inhibit lithium dendrite formation and mitigate volume expansion, demonstrating a significantly extended and consistent lifespan of 800 cycles (1600 h) at 1 mA cm−2 with low overpotential and insignificant voltage fluctuation for the process of lithium stripping and plating in symmetric cells. Herein, it is aimed to examine the transitions of metal oxides as a lithiophilic site for the lithium metal anode. It offers novel perspectives and approaches for the design of dendrite‐free lithium metal anodes. [ABSTRACT FROM AUTHOR]

Atomically dispersed metal‐nitrogen‐carbon catalysts have been extensively explored for various sustainable energy‐related reactions. From a material perspective, these catalysts are likely to consist of a combination of single‐atom, dual‐atom and possibly even multi‐atom sites. However, pinpointing their true active sites has remained a challenging task. In this study, a model catalyst is introduced, Co/CoMn‐NC, featuring both Co single‐atom sites and CoMn dual‐atom sites on a nitrogen‐doped carbon substrate. By employing a combination of X‐ray adsorption spectroscopy and density functional theory calculations, the atomic configuration of Co/CoMn‐NC has been determined. Density functional theory calculations are also used to unequivocally identify Co‐atom within the CoMn dual‐atom motif as the predominate active site of the Co/CoMn‐NC model catalyst toward oxygen reduction reaction (ORR), which is further confirmed by in situ Raman spectroscopy. The cooperative interactions between Co single‐atom sites and CoMn dual‐atom sites can finely tune the d‐band center and ameliorate the adsorption and desorption behaviors of the intermediates, thereby facilitating ORR kinetic. Overall, the study introduces a systematic strategy to elucidate the structure and the superiority of the model system and provides new insights into atomically dispersed multi‐metal active sites, showcasing that enhanced catalytic performance extends beyond unified diatomic sites or monatomic sites. [ABSTRACT FROM AUTHOR]

The water‐soluble salt‐template technique holds great promise for fabricating 3D porous materials. However, an equipment‐free and pore‐size controllable synthetic approach employing salt‐template precursors at room temperature has remained unexplored. Herein, we introduce a green room‐temperature antisolvent precipitation strategy for creating salt‐template self‐assembly precursors to universally produce 3D porous materials with controllable pore size. Through a combination of theoretical simulations and advanced characterization techniques, we unveil the antisolvent precipitation mechanism and provide guidelines for selecting raw materials and controlling the size of precipitated salt. Following the calcination and washing steps, we achieve large‐scale and universal production of 3D porous materials and the recycling of the salt templates and antisolvents. The optimized nitrogen‐doped 3D porous carbon (N‐3DPC) materials demonstrate distinctive structural benefits, facilitating a high capacity for potassium‐ion storage along with exceptional reversibility. This is further supported by in situ electrochemical impedance spectra, in situ Raman spectroscopy, and theoretical calculations. The anode shows a high rate capacity of 181 mAh g−1 at 4 A g−1 in the full cell. This study addresses the knowledge gap concerning the room‐temperature synthesis of salt‐template self‐assembly precursors for the large‐scale production of porous materials, thereby expanding their potential applications for electrochemical energy conversion and storage. [ABSTRACT FROM AUTHOR]

The water‐soluble salt‐template technique holds great promise for fabricating 3D porous materials. However, an equipment‐free and pore‐size controllable synthetic approach employing salt‐template precursors at room temperature has remained unexplored. Herein, we introduce a green room‐temperature antisolvent precipitation strategy for creating salt‐template self‐assembly precursors to universally produce 3D porous materials with controllable pore size. Through a combination of theoretical simulations and advanced characterization techniques, we unveil the antisolvent precipitation mechanism and provide guidelines for selecting raw materials and controlling the size of precipitated salt. Following the calcination and washing steps, we achieve large‐scale and universal production of 3D porous materials and the recycling of the salt templates and antisolvents. The optimized nitrogen‐doped 3D porous carbon (N‐3DPC) materials demonstrate distinctive structural benefits, facilitating a high capacity for potassium‐ion storage along with exceptional reversibility. This is further supported by in situ electrochemical impedance spectra, in situ Raman spectroscopy, and theoretical calculations. The anode shows a high rate capacity of 181 mAh g−1 at 4 A g−1 in the full cell. This study addresses the knowledge gap concerning the room‐temperature synthesis of salt‐template self‐assembly precursors for the large‐scale production of porous materials, thereby expanding their potential applications for electrochemical energy conversion and storage. [ABSTRACT FROM AUTHOR]

Noble metal Pt‐based catalysts have slow water dissociation kinetics at high pH conditions, making it difficult for water molecules to be electrochemically activated. Utilizing ligand effect and strain effect to tailor catalytic active sites is a common method, while the understanding of mechanism of their interaction remains obscure due to the complexity of the process. This study proposes a pulse‐induced torsional strained PtRu mesocrystals (PtRu MCs) with 20 times higher mass activity than commercial Pt/C. The combination of experimental results and theoretical calculations reveals that the ligand effect induced by Ru doping accelerates the kinetics of the water dissociation reaction, while the pulse‐induced torsion strained dominates the thermodynamic optimization of the hydrogen adsorption reaction. The structure‐activity relationship defined by the synergistic effect under the complementary advantages of the strain and doping provides guidance for the design of future basic hydrogen evolution catalysts. The catalyst can run stably at 1 A cm−2 for 500 h, showing potential for industrial application. [ABSTRACT FROM AUTHOR]

Atomically precise composite site‐based catalysts with new electrocatalytic synergistic mechanisms and enhanced electrocatalytic activities have emerged as a frontier in the electrocatalysis community. This topical review focuses on the recent research advances of atomically precise metal composite sites‐based electrocatalysts. This work first demonstrates an overview of the configurations of atomically precise composite sites, including a discussion of the advanced methods employed for understanding the composite sites. The review then provides a comprehensive organization of the previously reported methodologies of synthesizing electrocatalysts with atomically precise composite sites. Representative case studies are provided, starting from the simple one‐step pyrolysis strategy to the species‐by‐species multi‐step pyrolysis strategy. Based on the preceding discussions of the catalyst materials, the review further discusses the unique electrocatalysis mechanisms raised by the composite sites, that are different from the routine single species sites. The electrocatalytic systems mainly involve the oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, nitrogen reduction reaction, and carbon dioxide reduction reaction. The themes of this section include the true active center determination for composite sites and various types of electrocatalytic synergy mechanisms. Finally, critical unanswered questions and remaining challenges, as well as promising underexplored research directions are identified. [ABSTRACT FROM AUTHOR]

With more renewable energy developed to satisfy the human need in the energy crisis, electricity storage is critical in power utilization and storage. Due to its high safety, high nature reserve, and high energy density, the zinc‐based battery is drawing increasing attention. Together with the expansion of human activities, the low‐temperature battery is developed to satisfy the power demand in extreme environments, and as a critical component, electrolytes shall have a low freezing point and satisfying electrochemical properties in cold conditions. In this review, the development of low‐temperature electrolytes for zinc‐based batteries will be comprehensively introduced. First, the failure mechanism of zinc‐based battery at low temperature will be illustrated. Second, five main types of low‐temperature electrolytes will be introduced in detail. Finally, the regulation of electrolyte/electrode surface at low temperature will be discussed. This review aims to provide a guideline for low‐temperature electrolyte design from the perspective of molecular behavior regulation. [ABSTRACT FROM AUTHOR]

Rational design of Pt single‐atom catalysts provides a promising strategy to significantly improve the electrocatalytic activity for hydrogen evolution reaction. In this work, we presented a novel and efficient strategy for utilizing the low electron‐density region of substrate to effectively trap and confine high electron‐density metal atoms. The Pt single‐atom catalyst supported by nickel selenide with rich vacancies was prepared via a hydrothermal‐impregnation stepwise approach. Through experimental testation and DFT theoretical calculation, we confirm that Pt single atoms are well distributed at cationic vacancies of nickel selenide with loading amount of 3.2 wt. %. Moreover, the atomic Pt combined with the high electronegative Se to form Pt−Se bond as a "bridge" between single atoms and substrate for fast electron translation. This novel catalyst shows an extremely low overpotential of 45 mV at 10 mA cm−2 and an excellent stability over 120 h. Furthermore, the nickel selenide supported Pt SACs exhibits long‐term stability for practical application, which maintains a high current density of 390 mA cm−2 over 80 h with a retention of 99 %. This work points a promising direction for designing single atoms catalysts with high catalytic activity and stability for advanced green energy conversion technologies. [ABSTRACT FROM AUTHOR]

Rational design of Pt single‐atom catalysts provides a promising strategy to significantly improve the electrocatalytic activity for hydrogen evolution reaction. In this work, we presented a novel and efficient strategy for utilizing the low electron‐density region of substrate to effectively trap and confine high electron‐density metal atoms. The Pt single‐atom catalyst supported by nickel selenide with rich vacancies was prepared via a hydrothermal‐impregnation stepwise approach. Through experimental testation and DFT theoretical calculation, we confirm that Pt single atoms are well distributed at cationic vacancies of nickel selenide with loading amount of 3.2 wt. %. Moreover, the atomic Pt combined with the high electronegative Se to form Pt−Se bond as a "bridge" between single atoms and substrate for fast electron translation. This novel catalyst shows an extremely low overpotential of 45 mV at 10 mA cm−2 and an excellent stability over 120 h. Furthermore, the nickel selenide supported Pt SACs exhibits long‐term stability for practical application, which maintains a high current density of 390 mA cm−2 over 80 h with a retention of 99 %. This work points a promising direction for designing single atoms catalysts with high catalytic activity and stability for advanced green energy conversion technologies. [ABSTRACT FROM AUTHOR]

MXenes are promising substrates for supported noble metal electrocatalysts. Yet, it is a significant challenge to modulate the metal–support interaction (MSI) for enhancing catalytic performance. Herein, employing a facile HF etching method, the cation vacancy structures in Ti3C2Tx MXenes are controllably tuned, producing nearly vacancy‐free (Ti3C2Tx‐V0), single Ti atom vacancy (Ti3C2Tx‐VS), or Ti vacancy cluster (Ti3C2Tx‐VC) engineered MXenes. Ruthenium atomic clusters, as a model catalyst, successfully anchor on all MXene substrates. Different from the terminal O/F coordination groups on routine Ti3C2Tx MXene surfaces, the Ti vacancy clusters in Ti3C2Tx‐VC create unique lattice carbon ligand environment toward Ru species, which induces ultra‐strong MSI. As a result, compared to Ti3C2Tx‐V0 and Ti3C2Tx‐VS, the Ti3C2Tx‐VC modulated Ru clusters (Ru@Ti3C2Tx‐VC) exhibit the optimized balance of H2O adsorption/dissociation and OH/H desorption, thereby delivering superior electrocatalytic performance in the alkaline hydrogen evolution reaction (HER). Within the wide range from laboratory‐level (90 mA cm−2) to industrial‐level (1.5 A cm−2) current density, Ru@Ti3C2Tx‐VC outperforms commercial Pt/C in terms of overpotential and mass activity. Moreover, as a universal substrate for noble metal catalysts, Ti3C2Tx‐VC can also anchor Ir/Pt/Rh atomic clusters and enable excellent HER catalytic activity. This work expands the scope of the MSI between MXene and noble metal catalysts. [ABSTRACT FROM AUTHOR]

The sluggish kinetics and mutual interference of oxygen evolution and reduction reactions in the air electrode resulted in large charge/discharge overpotential and low energy efficiency of Zn‐air batteries. In this work, we designed a breathing air‐electrode configuration in the battery using P‐type Ca3Co4O9 and N‐type CaMnO3 as charge and discharge thermoelectrocatalysts, respectively. The Seebeck voltages generated from thermoelectric effect of Ca3Co4O9 and CaMnO3 synergistically compensated the charge and discharge overpotentials. The carrier migration and accumulation on the cold surface of Ca3Co4O9 and CaMnO3 optimized the electronic structure of metallic sites and thus enhanced their intrinsic catalytic activity. The oxygen evolution and reduction overpotentials were enhanced by 101 and 90 mV, respectively, at temperature gradient of 200 °C. The breathing Zn‐air battery displayed a remarkable energy efficiency of 68.1 %. This work provides an efficient avenue towards utilizing waste heat for improving the energy efficiency of Zn‐air battery. [ABSTRACT FROM AUTHOR]

The sluggish kinetics and mutual interference of oxygen evolution and reduction reactions in the air electrode resulted in large charge/discharge overpotential and low energy efficiency of Zn‐air batteries. In this work, we designed a breathing air‐electrode configuration in the battery using P‐type Ca3Co4O9 and N‐type CaMnO3 as charge and discharge thermoelectrocatalysts, respectively. The Seebeck voltages generated from thermoelectric effect of Ca3Co4O9 and CaMnO3 synergistically compensated the charge and discharge overpotentials. The carrier migration and accumulation on the cold surface of Ca3Co4O9 and CaMnO3 optimized the electronic structure of metallic sites and thus enhanced their intrinsic catalytic activity. The oxygen evolution and reduction overpotentials were enhanced by 101 and 90 mV, respectively, at temperature gradient of 200 °C. The breathing Zn‐air battery displayed a remarkable energy efficiency of 68.1 %. This work provides an efficient avenue towards utilizing waste heat for improving the energy efficiency of Zn‐air battery. [ABSTRACT FROM AUTHOR]

The advent of wearable electronics has strongly stimulated advanced research into the exploration of flexible zinc−air batteries (ZABs) with high theoretical energy density, high inherent safety, and low cost. However, the half‐open battery structure and the high concentration of alkaline aqueous environment pose great challenges on the electrolyte retention capability and the zinc anode stability. Herein, a starch‐based superabsorbent hydrogel polymer electrolyte (SSHPE) with high ionic conductivity, electrolyte absorption and retention capabilities, strong alkaline resistance and high zinc anode stability has been designed and applied in ZABs. Experimental and calculational analyses probe into the root of the superiority of SSHPEs, confirming the significance of the carboxyl functional groups along their polymer chains. These features endow the as‐fabricated ZAB a long cycle life of 300 h, much longer than that with commonly used poly(vinyl alcohol)‐based electrolyte. [ABSTRACT FROM AUTHOR]

The advent of wearable electronics has strongly stimulated advanced research into the exploration of flexible zinc−air batteries (ZABs) with high theoretical energy density, high inherent safety, and low cost. However, the half‐open battery structure and the high concentration of alkaline aqueous environment pose great challenges on the electrolyte retention capability and the zinc anode stability. Herein, a starch‐based superabsorbent hydrogel polymer electrolyte (SSHPE) with high ionic conductivity, electrolyte absorption and retention capabilities, strong alkaline resistance and high zinc anode stability has been designed and applied in ZABs. Experimental and calculational analyses probe into the root of the superiority of SSHPEs, confirming the significance of the carboxyl functional groups along their polymer chains. These features endow the as‐fabricated ZAB a long cycle life of 300 h, much longer than that with commonly used poly(vinyl alcohol)‐based electrolyte. [ABSTRACT FROM AUTHOR]

Alloying platinum with early transition metals is a promising approach to optimize the adsorption behaviors of catalysts. Nevertheless, the large negative redox potential between early transition metals and Pt hinders the fabrication of such alloys. Herein, a strategy combining the thermal shock technique with electrochemical activation to prepare Pt3V alloy as a hydrogen evolution reaction catalyst is reported for the first time. Electrochemical tests show that the as‐prepared catalyst exhibits exceptional catalytic activity and durability in 0.5 m H2SO4, surpassing the state‐of‐the‐art 20 wt.% Pt/C. The catalyst can maintain its activity after 100 h tests without evident decay under the current density of 500 mA cm−2. Theoretical calculations demonstrate that the optimized hydrogen absorption and high vacancy formation energy of Pt3V contributes to the enhanced electrocatalytic activity and stability. This work may spur future research for other Pt‐based early transition metal alloy catalysts for electrocatalysis. [ABSTRACT FROM AUTHOR]

It is vitally important to develop highly active, robust and low‐cost transition metal‐based electrocatalysts for overall water splitting in neutral solution especially at large current density. In this work, amorphous Mo‐doped NiS0.5Se0.5 nanosheets@crystalline NiS0.5Se0.5 nanorods (Am−Mo−NiS0.5Se0.5) was synthesized using a facil one‐step strategy. In phosphate buffer saline solution, the Am−Mo−NiS0.5Se0.5 shows tiny overpotentials of 48 and 209 mV for hydrogen evolution reaction (HER), 238 and 514 mV for oxygen evolution reaction (OER) at 10 and 1000 mA cm−2, respectively. Moreover, Am−Mo−NiS0.5Se0.5 delivers excellent stability for at least 300 h without obvious degradation. Theoretical calculations revealed that the Ni sites in the defect‐rich amorphous structure of Am−Mo−NiS0.5Se0.5 owns higher electron state density and strengthened the binding energy of H2O, which will optimize H adsorption/desorption energy barriers and reduce the adsorption energy of OER determining step. [ABSTRACT FROM AUTHOR]

The state‐of‐the‐art active hydrogen evolution reaction (HER) catalysts in acid electrolytes generally lose considerable catalytic performance in alkaline electrolytes mainly due to the additional water dissociation step. Designing composite materials is an effective strategy to accelerate alkaline water electrolysis by optimizing the electronic structure of materials. Here, different phases of Co(OH)2‐supported Ru clusters (α/β‐Co(OH)2@Ru) are prepared for enabling a highly efficient electrocatalytic HER performance in alkaline solution. The prepared α‐Co(OH)2 nanosheets facilitate the loading of uniform and high‐density Ru clusters and the formed highly active RuOCo bonds at the interface. The synergistic interaction endows the hybrid catalyst with low overpotential of 33 mV at 10 mA cm−2. Moreover, the homemade anion exchange membrane water electrolysis cell based on α‐Co(OH)2@Ru affords a cell voltage of 2 V to drive a current density of 270 mA cm−2 and performs stably during continuous operation for over 100 h. Density functional theory calculations demonstrate that active RuOCo bonds in α‐Co(OH)2@Ru optimize the energy barriers for H2O dissociation and OH− desorption to facilitate the Volmer reaction step. This work offers a strategy for designing interfacial chemical bonds for high electrocatalytic activity. [ABSTRACT FROM AUTHOR]

It is vitally important to develop highly active, robust and low‐cost transition metal‐based electrocatalysts for overall water splitting in neutral solution especially at large current density. In this work, amorphous Mo‐doped NiS0.5Se0.5 nanosheets@crystalline NiS0.5Se0.5 nanorods (Am−Mo−NiS0.5Se0.5) was synthesized using a facil one‐step strategy. In phosphate buffer saline solution, the Am−Mo−NiS0.5Se0.5 shows tiny overpotentials of 48 and 209 mV for hydrogen evolution reaction (HER), 238 and 514 mV for oxygen evolution reaction (OER) at 10 and 1000 mA cm−2, respectively. Moreover, Am−Mo−NiS0.5Se0.5 delivers excellent stability for at least 300 h without obvious degradation. Theoretical calculations revealed that the Ni sites in the defect‐rich amorphous structure of Am−Mo−NiS0.5Se0.5 owns higher electron state density and strengthened the binding energy of H2O, which will optimize H adsorption/desorption energy barriers and reduce the adsorption energy of OER determining step. [ABSTRACT FROM AUTHOR]

Supercapacitor (SC) is one of the most promising electrochemical energy‐storage devices. However, the practical application of SCs is limited by the low‐energy density. Herein, high‐temperature shock (HTS)‐derived ultrafine structure‐activated porous carbon (UAPC) with N, O functional groups is reported as high‐energy density SCs carbon. The process of ultrafast joule heating and cooling effectively transfers general‐purposed carbon into electrochemical‐activated carbon. The UAPC‐based SCs exhibit an energy density of up to 129 Wh kg−1 in EMIMBF4 ionic liquid, which outperform almost all reported and commercial SCs (22 Wh kg−1). The outstanding electrochemical performance of UAPC is attributed to the ultrafine structure and N, O functional groups, which enlarges the surface area, improves the surface wettability of UAPC electrodes, and provides pseudocapacitance. The facile and efficient ultrafast‐processing strategy has opened up an unprecedented pathway for the application of low‐value carbon for the electrode design and application of SCs. [ABSTRACT FROM AUTHOR]

Constructing novel heterostructures is an effective way for enhancing the oxygen electrocatalytic properties of the catalysts. In this work, a class of Janus homologous heterostructures, compositing transition metal alloys with their corresponding sulfides (TM/TMS), are controllably synthesized through an ultrafast high‐temperature shock (HTS) strategy. The ultrafast sintering rate and carbothermal reduction reaction lead to the formation of sulfides and partial reduction of sulfides to alloys, while the ultrafast cooling rate keeps the homologous heterostructure of TM/TMS stable. The components of TMs in the composites can be well controlled from unary to quaternary. Moreover, benefiting from the synergistic effect of the metallic sites in the interfaces, the adsorption and desorption energy barrier of the active intermediates are significantly optimized and thus leading to the enhanced oxygen catalytic performance. Impressively, the aqueous zinc‐air battery (ZAB) using the binary homologous nanocomposite FeCo/(FeCo)S as air cathodes achieves impressive durability (> 470 cycles) and power density (261.8 mW cm−2). The as‐assembled flexible ZAB can well power the wearable devices and can work for at least 300 cycles without obvious degradation. This work opens a new chemical space for designing homologous heterostructures for their application in energy storage and conversion systems. [ABSTRACT FROM AUTHOR]

Ion exchange membranes (IEMs) play important roles in energy generation and storage field, such as fuel cell, flow battery, however, a major barrier in the way of large‐scale application is the high cost of membranes (e.g., Nafion membranes price generally exceeds USD$ 200 m−2). The membrane‐less technology is one of the promising approaches to solve the problem and thus has attracted much attention and been explored in a variety of research paths. This review introduces one of the representative membrane‐less battery types, Biphasic membrane‐less redox batteries that eliminate the IEMs according to the principle of solvent immiscibility and realizes the phase splitting in a thermodynamically stable state. It is systematically classified and summarizes their performances as well as the problems they are suffering from, and then several effective solutions are proposed based on the modification of electrodes and electrolytes. Finally, special attention is given to the challenges and prospects of Biphasic membrane‐less redox batteries, which could contribute to the development of membrane‐less batteries. [ABSTRACT FROM AUTHOR]

Facilitating the cleavage of a NN bond and suppressing the competition hydrogen evolution reaction is essential, and but still remains a challenge in nitrogen reduction reaction (NRR). Crystal phase tailoring is an effective approach to optimize the energy barrier during the NRR process to improve the catalytic efficiency. Herein, a boron‐doping strategy to induce phase transfer from hexagonal Mo2C to cubic Mo2C for regulating the electronic structure and catalytic properties of electrocatalysts toward NRR is reported. The B doped cubic Mo2C is found to increase the exposure of active sites, regulate the d band center of Mo for enhancing the adsorption and activation of nitrogen, and reduce the energy barrier of NRR pathway, giving rise to a high ammonia yield of 52.1 μg h−1 mg−1 at −0.6 V versus reversible hydrogen electrode under ambient conditions. More importantly, the hydrogen adsorption on the surface of electrocatalyst is significantly inhibited due to the B‐doping, further improving the faradic efficiency to 36.9%, which is 4 times that of hexagonal Mo2C (9%). This work not only sheds light on the atomic‐scale design of efficient NRR electrocatalysts, but also provides a promising avenue for synchronizing the catalytic activity and selectivity for catalytic reactions. [ABSTRACT FROM AUTHOR]

Transition metal chalcogenides (TMCs) have been identified as pre‐electrocatalysts for the oxygen evolution reaction (OER) and the high valent TMs in the in situ generated oxyhydroxides are considered to be the real OER catalytic center. However, the role of chalcogens for OER process has been ignored and not fully elucidated. Herein, it is discovered that about 2.8–3.5% of chalcogens remain in as oxidized derivatives at a steady state, which plays a vital role for enhancing the catalytic activity. A facile and spontaneous sulfurizing method is developed to synthesize sulfur‐doped NiCo‐(oxy)hydroxysulfides (NCOSH) nanosheets, in which the sulfur can directly bond with high‐valence TMs and keep them stable for OER catalysis. Theoretical and experimental results suggest that the S‐coordination in NCOSH can cause bond length strengthening and electronic modulation between TM‐S and TM‐O, thus enhancing the oxidation activity and stability of high‐valence TMs in NCOSH. Consequently, the as‐obtained NCOSH exhibits superior bifunctional activities and durability for oxygen electrocatalytic reactions, and also serves as a superb air cathode in rechargeable solid state Zn‐air batteries. This work sheds light on the rational design of (oxy)hydroxysulfides as efficient electrocatalysts and gains deeper fundamental insights on the enhancing mechanism of S in oxyhydroxysulfides for diverse electrochemical applications. [ABSTRACT FROM AUTHOR]

The construction of binary metal Pd‐based catalysts is an effective strategy to enhance the activity of methanol oxidation reaction. Herein, atomically dispersed Ir single atoms doped to cuboctahedral Pd nanoparticles (Ir‐SAs/Pd) as efficient catalysts for alkaline methanol oxidation are prepared via a simple chemical reduction method. The synthetic Ir‐SAs/Pd catalysts exhibit the outstanding mass activity of about 1717.3 mA mgPd−1 compared with pure Pd and commercial Pd/C in electrooxidation for methanol. Meanwhile, the introduction of Ir single atoms enhances the CO tolerance of Pd nanoparticles to a large extent. On the basis of density functional theory results, the enhanced catalytic performance and CO tolerance rely on the effective improvement of the electron dominance near Fermi level and the negative shift of the d‐band center for Pd as a result of the electron redistribution between Pd and Ir atoms. This article will provide new insight into the design of high‐performance binary metal catalysts for methanol oxidation in alkaline media. [ABSTRACT FROM AUTHOR]

Improving Pt catalytic activity and minimizing its usage as well as enhancing its stability is highly desirable for oxidation of methanol and ammonia in the field of electrocatalysis. Herein, the nanoporous Pt with coral‐like nanowires morphology/carbon fiber cloth electrocatalyst is reported, which is synthesized via a simple electrodeposition approach using phytantriol lyotropic liquid crystals as template. The obtained electrode with 3D coral‐like Pt nanowires architecture is composed of the orderly in situ grown Pt nanowires, and each individual Pt nanowire possesses a large number of nanopores. As expected, coral‐like Pt nanowires electrodes possess high electrochemical surface area of 43.1 m2 g‐1, almost twice that (25.4 m2 g‐1) of commercial Pt/C, and thus display superior catalytic activity of 343.1 mA mg‐1 and 72.0 mA mg‐1 toward methanol and ammonia oxidation, much higher than that of the commercial Pt/C (173.7 mA mg‐1 and 26.2 mA mg‐1), respectively. Additionally, the retention rates of oxidation peak current of coral‐like Pt nanowires electrode toward both methanol and ammonia oxidation after accelerated 100 cycles test achieve 82.1% and 85.6%, respectively, indicating the excellent stability of coral‐like Pt nanowires electrode. [ABSTRACT FROM AUTHOR]

Abundant surface structural defects can endow electrocatalysts with extraordinary physical and chemical characteristics. Herein, metastable Pd nanoparticles (NPs) with abundant twin boundaries (TBs) and atomic steps (ASs) anchored on a carbon substrate (TS‐Pd/C) are directly synthesized by a solid‐state thermal shock (TS) strategy. Molecular dynamics simulation indicates that the transient super cooling procedure after the TS synthesis can boost the formation of TBs. Benefitting from the abundant TBs and ASs, these metastable Pd NPs can serve as an advanced electrocatalyst for the ethanol oxidation reaction (EOR) with superior reactivity, stability, and CO tolerance in alkaline solutions, which far exceeds that of commercial Pd/C. The first‐principles calculations suggest that the defect structure dominated by TBs can achieve the spatial separation of the optimal adsorption sites for CO and OH. The CO can concentrate at optimal surface sites to minimize the number of poisoned active sites. The strong adsorption of OH can accelerate the EOR process and jointly promote the improvement of electrocatalytic reactivity. [ABSTRACT FROM AUTHOR]

Owing to its unique atomic arrangement and electronic structure, metallic glass (MG) has been widely investigated in the field of energy storage and conversion. In the past few decades, multiple strategies have been developed to synthesize bulk and nanosized MG based materials. Here, combining the structure–activity relationship of MG with electrochemical reaction kinetics, the substantial progress of glass structures in electrocatalytic processes are highlighted, including the hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, methanol oxidation reaction, carbon dioxide reduction reaction, and nitrogen fixation. Meanwhile, applications of MG materials in energy storage devices, like supercapacitors and lithium‐ion batteries, are also introduced in detail. Finally, challenges and possibilities for reasonable design of highly‐efficient MG‐based electrode materials are proposed. The integration of high‐throughput methods, artificial intelligence technology, as well as advanced characterization techniques is fundamental to screen materials with remarkable performance. This review aims to deepen the understanding of the relationship between electronic structure and electrochemical performance, providing guidance for rational design of functional MG materials with outstanding activity, selectivity, and durability. [ABSTRACT FROM AUTHOR]

The development of new catalysts is an urgent task in chemistry research because of the increasing demands for higher productivity and efficiency in modern industrial chemistry. High‐throughput (HT) technologies have emerged as powerful accelerators for the discovery of new catalytic materials. Generally, HT techniques involve HT computational screening of catalytic materials and HT experimental approaches. Significant progress has been made in discovering and optimizing catalysts, which demonstrates the speed and economic advantages of HT methods in a matter of process within days and even hours, in contrast with traditional time‐consuming trial and error experiments. From this perspective, the key processes of HT technologies for building a catalysts library are highlighted, including the virtual lab construction based on informatics tools and experimental data lab involving the following processes: 1) design of experiments; 2) reactants prepared manually or automatically; 3) constructing reactor that can well control the variations including materials diversity and reaction conditions (e.g., temperature and reaction time); 4) parallel characterization of fabricated catalysts. Moreover, the correlation between virtual lab and experimental data is discussed to inspire explorations in this field. Furthermore, several remaining challenges of HT technologies accompanied by possible research directions are presented to promote efforts in catalysts library creation. [ABSTRACT FROM AUTHOR]

Rational design of bifunctional efficient electrocatalysts for both oxygen reduction (ORR) and oxygen evolution reactions (OER) is desirable—while highly challenging—for development of rechargeable metal–air batteries. Herein, an efficient bifunctional electrocatalyst is designed and fabricated by encapsulating Co nanoparticles in interconnected N‐doped hollow porous carbon nanofibers (designated as Co@N‐C/PCNF) using an ultrafast high‐temperature shock technology. Benefiting from the synergistic effect and intrinsic activity of the CoNC moiety, as well as porous structure of carbon nanofibers, the Co@N‐C/PCNF composite shows high bifunctional electrocatalytic activities for both OER (289 mV at 10 mA cm−2) and ORR (half‐wave potential of 0.85 V). The CoNC moiety in the composite can modulate the local environmental and electrical structure of the catalysts, thus optimizing the adsorption/desorption kinetics and decreasing the reaction barriers for promoting the reversible oxygen electrocatalysis. Co@N‐C/PCNF‐based aqueous Zn–air batteries (AZAB) provide high power density of 292 mW cm−2, and the assembled flexible ZAB can power wearable devices. [ABSTRACT FROM AUTHOR]

With the low redox potential of −3.04 V (vs SHE) and ultrahigh theoretical capacity of 3862 mAh g−1, lithium metal has been considered as promising anode material. However, lithium metal battery has ever suffered a trough in the past few decades due to its safety issues. Over the years, the limited energy density of the lithium‐ion battery cannot meet the growing demands of the advanced energy storage devices. Therefore, lithium metal anodes receive renewed attention, which have the potential to achieve high‐energy batteries. In this review, the history of the lithium anode is reviewed first. Then the failure mechanism of the lithium anode is analyzed, including dendrite, dead lithium, corrosion, and volume expansion of the lithium anode. Further, the strategies to alleviate the lithium anode issues in recent years are discussed emphatically. Eventually, remaining challenges of these strategies and possible research directions of lithium‐anode modification are presented to inspire innovation of lithium anode. [ABSTRACT FROM AUTHOR]

Tuning the electronic states near the Fermi level can effectively facilitate the reaction kinetics. However, elucidating the role of a specific electronic state of metal oxide in simultaneously regulating the CO2 electroreduction reaction (CO2RR) and competing hydrogen evolution reaction (HER) is still rare, making it difficult to accurately predict the practical CO2RR performance. Herein, replacing the Zn site by heteroatoms with different outer electrons (Mo and Cu) is found to tune both occupied and unoccupied orbitals near the Fermi level of ZnO. Moreover, the different electronic states significantly modulate both CO2RR and HER activity with a totally inverse trend, thus dramatically tuning the practical CO2RR performance. In parallel, the correlation between electronic states, reaction free energies and practical activity is demonstrated. This work provides a possibility for engineering efficient CO2RR eletrocatalysts through tunable composition and electronic structures. [ABSTRACT FROM AUTHOR]

Tuning the electronic states near the Fermi level can effectively facilitate the reaction kinetics. However, elucidating the role of a specific electronic state of metal oxide in simultaneously regulating the CO2 electroreduction reaction (CO2RR) and competing hydrogen evolution reaction (HER) is still rare, making it difficult to accurately predict the practical CO2RR performance. Herein, replacing the Zn site by heteroatoms with different outer electrons (Mo and Cu) is found to tune both occupied and unoccupied orbitals near the Fermi level of ZnO. Moreover, the different electronic states significantly modulate both CO2RR and HER activity with a totally inverse trend, thus dramatically tuning the practical CO2RR performance. In parallel, the correlation between electronic states, reaction free energies and practical activity is demonstrated. This work provides a possibility for engineering efficient CO2RR eletrocatalysts through tunable composition and electronic structures. [ABSTRACT FROM AUTHOR]

Construction of active and durable non‐noble‐metals based electrocatalysts is one of important requirements for the practical application and development of fuel cells, which are presently inhibited by relative sluggish charge transport and reaction kinetics. Herein, highly dispersed ultrathin carbon‐coated nickel oxide nanoparticles settled on carbon cloth (NiO@C/CC) as efficient catalysts for alkaline fuels oxidation are synthesized via an air‐assisted transient thermal shock strategy. This NiO@C/CC catalyst induces an outstanding catalytic activity (up to 119.1 mA cm−2) and durability (a little current decay during tests) in electrooxidation for ethanol, even for methanol and ethylene glycol, which outperforms most of the reported non‐noble metal catalysts. The excellent catalytic performance of NiO@C/CC is essentially attributed to the oxygen vacancies, high concentration, high‐valence‐state Ni, and carbon layers of NiO@C NPs, which contribute to regulate the surface properties and electronic structure, enhance charge transfer, and provide abundant active sites, promoting adsorption capacity of reactant molecules on its surface. The facile and promising air‐assisted transient thermal shock strategy can be extended to guide rational design and rapid synthesis of transition metal compounds as advanced catalysts for alkaline direct alcohol fuel cells. [ABSTRACT FROM AUTHOR]

Cu2O is a typical photoelectrocatalyst for sustainable hydrogen production, while the fast charge recombination hinders its further development. Herein, Ni2+ cations have been doped into a Cu2O lattice (named as Ni‐Cu2O) by a simple hydrothermal method and act as electron traps. Theoretical results predict that the Ni dopants produce an acceptor impurity level and lower the energy barrier of hydrogen evolution. Photoelectrochemical (PEC) measurements demonstrate that Ni‐Cu2O exhibits a photocurrent density of 0.83 mA cm−2, which is 1.34 times higher than that of Cu2O. And the photostability has been enhanced by 7.81 times. Moreover, characterizations confirm the enhanced light‐harvesting, facilitated charge separation and transfer, prolonged charge lifetime, and increased carrier concentration of Ni‐Cu2O. This work provides deep insight into how acceptor‐doping modifies the electronic structure and optimizes the PEC process. [ABSTRACT FROM AUTHOR]

Cu2O is a typical photoelectrocatalyst for sustainable hydrogen production, while the fast charge recombination hinders its further development. Herein, Ni2+ cations have been doped into a Cu2O lattice (named as Ni‐Cu2O) by a simple hydrothermal method and act as electron traps. Theoretical results predict that the Ni dopants produce an acceptor impurity level and lower the energy barrier of hydrogen evolution. Photoelectrochemical (PEC) measurements demonstrate that Ni‐Cu2O exhibits a photocurrent density of 0.83 mA cm−2, which is 1.34 times higher than that of Cu2O. And the photostability has been enhanced by 7.81 times. Moreover, characterizations confirm the enhanced light‐harvesting, facilitated charge separation and transfer, prolonged charge lifetime, and increased carrier concentration of Ni‐Cu2O. This work provides deep insight into how acceptor‐doping modifies the electronic structure and optimizes the PEC process. [ABSTRACT FROM AUTHOR]

Functional nanomaterials are playing a crucial role in the emerging field of energy‐related devices. Recently, as a novel synthesis method, high‐temperature shock (HTS), which is rapid, low cost, eco‐friendly, universal, scalable, and controllable, has provided a promising option for the rational design and synthesis of various high‐quality nanomaterials. In this report, the HTS technique, including the equipment setup and operating principle, is systematically introduced, and recent progress in the synthesis of nanomaterials for energy storage and conversion applications using this HTS method is summarized. The growth mechanisms of nanoparticles and carbonaceous nanomaterials are thoroughly discussed, followed by the summary of the characteristic advantages of the HTS strategy. A series of nanomaterials prepared by the HTS method, including carbon‐based films, metal nanoparticles and compound nanoparticles, show high performance in the diverse applications of storage energy batteries, highly active catalysts, and smart energy devices. Finally, the future perspectives and directions of HTS in nanomanufacturing for broader applications are presented. [ABSTRACT FROM AUTHOR]

Highly efficient electrocatalysts play an integral part in developing renewable energy conversion and storage technologies. Despite considerable efforts devoted to synthesizing electrocatalysts with superior performance, the identification of active moieties and understanding of reaction mechanisms under practical conditions still remain elusive. Herein, the substantial progresses in unraveling the local electronic and atomic structure optimizations of nanocatalysts for gas‐involved electrocatalysis, disclosing real active sites, and clarifying their relationships with intrinsic activities by combining advanced characterization techniques with computational simulations are summarized. The continuous development of in situ and ex situ characterization tools, particularly at multi‐scale resolution, to monitor or even directly observe the active center structure is systematically discussed, which is divided into four main categories based on the type of active sites: atomically dispersed active sites, vacancies, heteroatom doping sites, and edge sites. Current challenges and perspectives in both fundamental area and industrial application are finally proposed for the future research direction of next‐generation electrode materials. The aim of this review is to provide mechanistic insights into the real catalytically active structure with the assistance of newly developed characterization techniques, guiding the rational design and structure engineering of advanced functional materials with outstanding activity, selectivity, and durability. [ABSTRACT FROM AUTHOR]