Facilitating charge transfer via a Semi-Coherent Fe(PO3)2-Co2P2O7 heterointerface for highly efficient Zn-Air batteries.

Developing reversible oxygen electrodes for both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is crucial for achieving high-performance rechargeable Zn-air batteries (ZABs). This study introduced an nitrogen-doped carbon confined with a semi-coherent Fe(PO3)2-Co2P2O7 heterojunction for bifunctional oxygen electrocatalysis. This nanocomposite yielded an ORR half-wave potential of 0.908 V and an OER overpotential of 291 mV at 10 mA/cm2. ZABs incorporating this catalyst yielded impressive performance, including a peak power density of 203 mW/cm2, a specific capacity of 737 mAh/gZn, and promoted stability. Both experimental and theoretical simulations demonstrated that the unique electric field between Fe(PO3)2 and Co2P2O7 promoted efficient charge transport across the heterointerface. This interaction likely modulated the d-band center of the heterojunction, expedite the desorption of oxygen intermediates, thus improving oxygen catalysis and, consequently, ZAB performance. This work illustrates a significant design principle for creating efficient bifunctional catalysts in energy conversion technologies.

Surface crystallized supramolecular to achieve highly dispersed ultrafine nano-palladium in-situ deposition to promote thermal/electrocatalytic reduction.

To promote the greening and economization of industrial production, the development of advanced catalyst manufacturing technology with high activity and low cost is an indispensable part. In this study, nitrogen-doped hollow carbon spheres (NHCSs) were used as anchors to construct a supramolecular coating formed by the self-assembly of boron clusters and ß-cyclodextrin by surface crystallization strategy, with the help of the weak reducing agent characteristics of boron clusters, highly dispersed ultra-small nano-palladium particles were in-situ embedded on the surface of NHCSs. The deoxygenation hydrogenation of nitroaromatics and the reduction of nitrate to ammonia were used as the representatives of thermal catalytic reduction and electrocatalytic reduction respectively. The excellent properties of the constructed Pd/NHCSs were proved by the probe reaction. In the catalytic hydrogenation of nitroaromatics to aminoaromatics, the reaction kinetic rate and activation energy are at the leading level. At the same time, the constructed Pd/NHCSs can also electrocatalytically reduce nitrate to high value-added ammonia with high activity and selectivity, and the behavior of Pd/NHCSs high selectivity driving nitrate conversion was revealed by density functional theory and in situ attenuated total reflection Fourier transform infrared (ATRFTIR) technique. These results all reflect the feasibility and superiority of in-situ anchoring ultra-small nano-metals as catalysts by surface crystallization to build a supramolecular cladding with reducing properties, which is an effective way to construct high-activity and low-cost advanced catalysts.

Recent Advances in Antimony Selenide Photodetectors.

Photodetectors (PDs) rapidly capture optical signals and convert them into electrical signals, making them indispensable in a variety of applications including imaging, optical communication, remote sensing, and biological detection. Recently, antimony selenide (Sb2Se3) has achieved remarkable progress due to its earth-abundant, low toxicity, low price, suitable bandgap width, high absorption coefficient, and unique structural characteristics. Sb2Se3 has been extensively studied in solar cells, but there's a lack of timely updates in the field of PDs. A literature review based on Sb2Se3 PDs is urgently warranted. This review aims to provide a concise understanding of the latest progress in Sb2Se3 PDs, with a focus on the basic characteristics and the performance optimization for Sb2Se3 photoconductive-type and photodiode-type detectors, including nanostructure regulation, process optimization, and stability improvement of flexible devices. Furthermore, the application progresses of Sb2Se3 PDs in heart rate monitoring, and monolithic-integrated matrix images are introduced. Finally, this review presents various strategies with potential and feasibility to address challenges for the rapid development and commercial application of Sb2Se3 PDs.

Functional partitioning synergistically enhances multi-scenario nitrate reduction.

The promising electrocatalytic nitrate reduction reaction (eNitRR) for distributed ammonia synthesis requires the fine design of functionally compartmentalised and synergistically complementary integrated catalysts to meet the needs of low-cost and efficient ammonia synthesis. Herein, the partitionable CoP3 and Cu3P modules were built on the copper foam substrate, and the functional differentiation promoted the catalytic performance of the surface accordion-like CoP3/Cu3P@CF for eNitRR in complex water environment. Where the ammonia yield rate is as high as 23988.2 µg h-1 cm-2, and the Faradaic efficiency is close to 100 %. With CoP3/Cu3P@CF as the core, the assembled high-performance Zn-nitrate flow battery can realize the dual function of ammonia production and power supply, and can also realize the continuous production of ammonia with high selectivity driven by solar energy. The ammonia recovery reaches 753.9 mg L-1, which shows the superiority of CoP3/Cu3P@CF in multiple application scenarios and provides important experience for the vigorous development of eNitRR. Density functional theory calculation reveal that CoP3 and Cu3P sites play a relay synergistic role in eNitRR catalyzed by CoP3/Cu3P@CF. CoP3 first promotes the activation of NO3- to *NO3H, and then continuously provides proton hydrogen for the eNitRR on the surface of Cu3P, which relays the synergistic catalytic effect to promote the efficient conversion of NO3- to NH3. This study not only develops a catalyst that can promote the efficient reduction of NO3- to ammonia through an easy-to-obtain innovative strategy, but also provides an alternative strategy for the development of eNitRR that is suitable for multiple scenarios and meets the production conditions.

Enhanced Oxygen Evolution and Zinc-Air Battery Performance via Electronic Spin Modulation in Heterostructured Catalysts.

Beyond optimizing electronic energy levels, the modulation of the electronic spin configuration is an effective strategy, often overlooked, to boost activity and selectivity in a range of catalytic reactions, including the oxygen evolution reaction (OER). This electronic spin modulation is frequently accomplished using external magnetic fields, which makes it impractical for real applications. Herein, spin modulation is achieved by engineering Ni/MnFe2O4 heterojunctions, whose surface is reconstructed into NiOOH/MnFeOOH during the OER. NiOOH/MnFeOOH shows a high spin state of Ni, which regulates the OH- and O2 adsorption energy and enables spin alignment of oxygen intermediates. As a result, NiOOH/MnFeOOH electrocatalysts provide excellent OER performance with an overpotential of 261 mV at 10 mA cm-2. Besides, rechargeable zinc-air batteries based on Ni/MnFe2O4 show a high open circuit potential of 1.56 V and excellent stability for more than 1000 cycles. This outstanding performance is rationalized using density functional theory calculations, which show that the optimal spin state of both Ni active sites and oxygen intermediates facilitates spin-selected charge transport, optimizes the reaction kinetics, and decreases the energy barrier to the evolution of oxygen. This study provides valuable insight into spin polarization modulation by heterojunctions enabling the design of next-generation OER catalysts with boosted performance.

Pomelo peel biomass derived highly active advanced-oxidation-process catalyst: Complete elimination of organic pollutants.

The advanced oxidation process (AOPs) is playing an important role in the elimination of hazardous organic pollutants, but the development of inexpensive and highly active advanced catalysts is facing challenges. In this study, a low-cost and readily available agricultural waste resource pomelo peel-flesh (PPF) biomass was used as the basic raw material, and the uniformly dispersed small cobalt nanoparticles were effectively anchored in the biochar derived from pomelo peel-flesh (BDPPF) by impregnation adsorption/complexation combined with heat treatment. Co/BDPPF (BDPPF embedded with Co) can effectively activate peroxymonosulfate (PMS) to SO4·-, ·OH and 1O2 reactive oxygen species, and achieve nearly 100% degradation of tetracycline persistent organic pollutant. Co/BDPPF can not only degrade tetracycline efficiently in complex water environment, but also degrade most organic pollutants universally, and has long-term stability, which solves the problem of poor universality and stability of heterogeneous catalysts to a certain extent. Importantly, Co/BDPPF derived from waste biomass was also innovatively designed as the core of an integrated continuous purification device to achieve continuous purification of organic wastewater. In this study, agricultural waste resources were selected as biomass raw materials to achieve efficient capture of Co2+, and finally developed advanced AOPs catalyst with excellent performance to achieve the purification of organic wastewater. It also provides a promising solution for the preparation of simple, low-cost, large-scale production of AOPs catalysts that can be put into actual production.

C3N5-based nanomaterials and their applications in heterogeneous catalysts, energy harvesting, and environmental remediation.

Over the past few decades, the global reliance on fossil fuels and the exponential growth of human population have escalated global energy consumption and environmental issues. To tackle these dual challenges, metal catalysts, in particular precious metal ones, have emerged as pivotal players in the fields of environment and energy. Among the numerous metal-free and organic catalyst materials, C3N5-based materials have a major advantage over their carbon nitride (CxNy) counterparts owing to the abundant availability of raw materials, non-toxicity, non-hazardous nature, and exceptional performance. Although significant efforts have been dedicated to synthesising and optimising the applicable properties of C3N5-based materials in recent years, a comprehensive summary of the immediate parameters of this promising material is still lacking. Given the rapid development of C3N5-based materials, a timely review is essential for staying updated on their strengths and weaknesses across various applications, as well as providing guidance for designing efficient catalysts. In this study, we present an extensive overview of recent advancements in C3N5-based materials, encompassing their physicochemical properties, major synthetic methods, and applications in photocatalysis, electrocatalysis, and adsorption, among others. This systematic review effectively summarises both the advantages and shortcomings associated with C3N5-based materials for energy and environmental applications, thus offering researchers focussed on CxNy-materials an in-depth understanding of those based on C3N5. Finally, considering the limitations and deficiencies of C3N5-based materials, we have proposed enhancement schemes and strategies, while presenting personal perspectives on the challenges and future directions for C3N5. Our ultimate aim is to provide valuable insights for the research community in this field.

Subnanometric Osmium Clusters Confined on Palladium Metallenes for Enhanced Hydrogen Evolution and Oxygen Reduction Catalysis.

Highly efficient, cost-effective, and durable electrocatalysts, capable of accelerating sluggish reaction kinetics and attaining high performance, are essential for developing sustainable energy technologies but remain a great challenge. Here, we leverage a facile heterostructure design strategy to construct atomically thin Os@Pd metallenes, with atomic-scale Os nanoclusters of varying geometries confined on the surface layer of the Pd lattice, which exhibit excellent bifunctional properties for catalyzing both hydrogen evolution (HER) and oxygen reduction reactions (ORR). Importantly, Os5%@Pd metallenes manifest a low η10 overpotential of only 11 mV in 1.0 M KOH electrolyte (HER) as well as a highly positive E1/2 potential of 0.92 V in 0.1 M KOH (ORR), along with superior mass activities and electrochemical durability. Theoretical investigations reveal that the strong electron redistribution between Os and Pd elements renders a precise fine-tuning of respective d-band centers, thereby guiding adsorption of hydrogen and oxygen intermediates with an appropriate binding energy for the optimal HER and ORR.

A Full-Spectrum ZnS Photocatalyst with Gradient Distribution of Atomic Copper Dopants and Concomitant Sulfur Vacancies for Highly Efficient Hydrogen Evolution.

A rarely discussed phenomenon in the realm of photocatalytic materials involves the presence of gradient distributed dopants and defects from the interior to the surface. This intriguing characteristic has been successfully achieved in the case of ZnS through the incorporation of atomic monovalent copper ions (Cu+) and concurrent sulfur vacancies (Vs), resulting in a photocatalyst denoted as G-CZS1-x. Through the cooperative action of these atomic Cu dopants and Vs, G-CZS1-x significantly extends its photoabsorption range to encompass the full spectrum (200-2100 nm), which improves the solar utilization ability. This alteration enhances the efficiency of charge separation and optimizes Δ(H*) (free energy of hydrogen adsorption) to approach 0 eV for the hydrogen evolution reaction (HER). It is noteworthy that both surface-exposed atomic Cu and Vs act as active sites for photocatalysis. G-CZS1-x exhibits a significant H2 evolution rate of 1.01 mmol h-1 in the absence of a cocatalyst. This performance exceeds the majority of previously reported photocatalysts, exhibiting approximately 25-fold as ZnS, and 5-fold as H-CZS1-x with homogeneous distribution of equal content Cu dopants and Vs. In contrast to G-CZS1-x, the H adsorption on Cu sites for H-CZS1-x (ΔG(H*) = -1.22 eV) is excessively strong to inhibit the H2 release, and the charge separation efficiency for H-CZS1-x is relatively sluggish, revealing the positive role of a gradient distribution model of dopants and defects on activity enhancement. This work highlights the synergy of atomic dopants and defects in advancing photoactivity, as well as the significant benefit of the controllable distribution model of dopants and defects for photocatalysis.

Dipole Field-Driven Organic-Inorganic Heterojunction for Highly Sensitive Ultraviolet Photodetector.

Developing high-performance organic-inorganic ultraviolet (UV) photodetectors (PDs) has attracted considerable attention. However, this development has been hindered due to poor directional charge-transfer ratios in transport layers, excessive costs, and an ambiguous underlying mechanism. To tackle these challenges, we constructed a heterojunction of economic Mg-doped ZnO (MgZnO) nanorods and poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) [PEDOT:PSS (P:P)] that utilizes dipole field-driven spontaneous polarization to enhance photogenerated charge kinetics. As a result, the proposed heterojunction has an improved noise equivalent power of 3.16 × 10-11 W Hz-1/2), a normalized detection rate (D*) of 8.96 × 109 jones, and external quantum efficiency comparable to other ZnO-based devices. Notably, the prepared PDs showed a photocurrent of 4.8 × 10-3 µA under a faint UV light having an intensity of 1 × 10-5 W cm-2, exceeding the performance of the most state-of-the-art ZnO-based UV sensors. The introduction of Mg into ZnO is responsible for the high performance, as it causes a lattice mismatch and distortion of the Mg-doped ZnO unit cell. It results in improved dipole movement and the creation of a dipole field, accelerating the directional electron-transfer process. Using a dipole field to manipulate the migration and transport of photogenerated carriers represents a promising approach for achieving outstanding performance in UV PDs.

Recent Advances of Green Electricity Generation: Potential in Solar Interfacial Evaporation System.

Solar-driven interfacial evaporation (SDIE) has played a pivotal role in optimizing water-energy utilization, reducing conventional power costs, and mitigating environmental impacts. The increasing emphasis on the synergistic cogeneration of water and green electricity through SDIE is particularly noteworthy. However, there is a gap of existing reviews that have focused on the mechanistic understanding of green power from water-electricity cogeneration (WEC) systems, the structure-activity relationship between efficiency of green energy utilization in WEC and material design in SDIE. Particularly, it lacks a comprehensive discussion to address the challenges faced in these areas along with potential solutions. Therefore, this review aims to comprehensively assess the progress and future perspective of green electricity from WEC systems by investigating the potential expansion of SDIE. First, it provides a comprehensive overview about material rational design, thermal management, and water transportation tunnels in SDIE. Then, it summarizes diverse energy sources utilized in the SDIE process, including steaming generation, photovoltaics, salinity gradient effect, temperature gradient effect, and piezoelectric effect. Subsequently, it explores factors that affect generated green electricity efficiency in WEC. Finally, this review proposes challenges and possible solution in the development of WEC.

Unveiling Cutting-Edge Developments in Electrocatalytic Nitrate-to-Ammonia Conversion.

The excessive enrichment of nitrate in the environment can be converted into ammonia (NH3) through electrochemical processes, offering significant implications for modern agriculture and the potential to reduce the burden of the Haber-Bosch (HB) process while achieving environmentally friendly NH3 production. Emerging research on electrocatalytic nitrate reduction (eNitRR) to NH3 has gained considerable momentum in recent years for efficient NH3 synthesis. However, existing reviews on nitrate reduction have primarily focused on limited aspects, often lacking a comprehensive summary of catalysts, reaction systems, reaction mechanisms, and detection methods employed in nitrate reduction. This review aims to provide a timely and comprehensive analysis of the eNitRR field by integrating existing research progress and identifying current challenges. This review offers a comprehensive overview of the research progress achieved using various materials in electrochemical nitrate reduction, elucidates the underlying theoretical mechanism behind eNitRR, and discusses effective strategies based on numerous case studies to enhance the electrochemical reduction from NO3 - to NH3. Finally, this review discusses challenges and development prospects in the eNitRR field with an aim to guide design and development of large-scale sustainable nitrate reduction electrocatalysts.

ZIFs-Derived Hollow Nanostructures via a Strong/Weak Coetching Strategy for Long-Life Rechargeable Zn-Air Batteries.

Recently, zeolitic imidazolate frameworks (ZIFs) composites have emerged as promising precursors for synthesizing hollow-structured N-doped carbon-based noble-metal materials with diverse structures and compositions. Here, a strong/weak competitive coordination strategy is presented for synthesizing high-performance electrocatalysts with hollow features. During the competitive coordination process, the cubic zeolitic-imidazole framework-8 (Cube-8)@ZIF-67 with core-shell structures are transformed into Cube-8@ZIF-67@PF/POM with yolk-shell nanostructures employing phosphomolybdic acid (POM) and potassium ferricyanide (PF) as the strong chelator and the weak chelator, respectively. After calcination, the hollow Mo/Fe/Co@NC catalyst exhibits superior performance in both oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Interestingly, the Mo/Fe/Co@NC catalyst exhibits efficient electrocatalytic performance for Zn-air batteries (ZABs), with a high power density (≈150 mW cm-2) and superior cycling life (≈500 h) compared to commercial platinum/carbon (Pt/C) and ruthenium dioxide (RuO2) mixture benchmarks catalysts. In addition, the density functional theory further proves that after the introduction of Mo and Fe atoms, the adsorption energy with the adsorption intermediates is weakened by adjusting the d-band center, thus weakening the reaction barrier and promoting the reaction kinetics of OER. Undoubtedly, this study presents novel insights into the fabrication of ZIFs-derived hollow structure bifunctional oxygen electrocatalysts for clean-energy diverse applications.

Confining Bismuth-Halide Perovskite in Mesochannels of Silica Nanomembranes for Exceptional Photocatalytic Abatement of Air Pollutants.

Spatially confined photocatalysis has emerged as a viable strategy for the intensification of various redox reactions, but the influence of confined structure on reaction behavior is always overlooked in gas-solid reactions. Herein, we report a nanomembrane with confining Cs3 Bi2 Br9 nanocrystals inside vertical channels of porous insulated silica thin sheets (CBB@SBA(⊥)) for photocatalytic nitric oxide (NO) abatement. The ordered one-dimensional (1D) pore channels with mere 70 nm channel length provide a highly accessible confined space for catalytic reactions. A record-breaking NO conversion efficiency of 98.2 % under a weight hourly space velocity (WHSV) of 3.0×106  mL g-1 h-1 , as well as exceptionally high stability over 14 h and durability over a wide humidity range (RH=15-90 %) was realized over SBA(⊥) confined Cs3 Bi2 Br9 , well beyond its nonconfined analogue and the Cs3 Bi2 Br9 confine in Santa Barbara Amorphous (SBA-15). Mechanism studies suggested that the insulated pore channels of SBA(⊥) in CBB@SBA(⊥) endow concentrated electron field and enhanced mass transfer that render high exposure of reactive species and lower reaction barrier needs for ⋅O2 - formation and NO oxidation, as well as prevents structural degradation of Cs3 Bi2 Br9 . This work expands an innovative strategy for designing efficient photocatalysts for air pollution remediation.

Nitrogen-bridged Fe-Cu Atomic Pair Sites for Efficient Electrochemical Ammonia Production and Electricity Generation with Zn-NO2 Batteries.

The development of environmentally sustainable and highly efficient technologies for ammonia production is crucial for the future advancement of carbon-neutral energy systems. The nitrite reduction reaction (NO2 RR) for generating NH3 is a promising alternative to the low-efficiency nitrogen reduction reaction (NRR), owing to the low N=O bond energy and high solubility of nitrite. In this study, we designed a highly efficient dual-atom catalyst with Fe-Cu atomic pair sites (termed FeCu DAC), and the as-developed FeCu DAC was able to afford a remarkable NH3 yield of 24,526 µg h-1 mgcat. -1 at -0.6 V, with a Faradaic Efficiency (FE) for NH3 production of 99.88 %. The FeCu DAC also exhibited exceptional catalytic activity and selectivity in a Zn-NO2 battery, achieving a record-breaking power density of 23.6 mW cm-2 and maximum NH3 FE of 92.23 % at 20 mA cm-2 . Theoretical simulation demonstrated that the incorporation of the Cu atom changed the energy of the Fe 3d orbital and lowered the energy barrier, thereby accelerating the NO2 RR. This study not only demonstrates the potential of galvanic nitrite-based cells for expanding the field of Zn-based batteries, but also provides fundamental interpretation for the synergistic effect in highly dispersed dual-atom catalysts.

Tuning Coordination Structures of Zn Sites Through Symmetry-Breaking Accelerates Electrocatalysis.

Manipulating the coordination environment of individual active sites in a precise manner remains an important challenge in electrocatalytic reactions. Herein, inspired by theoretical predictions, a facile procedure to synthesize a series of symmetry-breaking zinc metal-organic framework (Zn-MOF) catalysts with well-defined structures is presented. Benefiting from the optimized coordination microenvironment regulated by symmetry-breaking, Zn-N2 S2 -MOF exhibits the best performance of nitrogen (N2 ) reduction reaction (NRR) with NH3 yield rate of 25.07 ± 1.57 µg h-1  cm-2 and Faradaic efficiency of 44.57 ± 2.79% compared with reported Zn-based NRR catalysts. X-ray absorption near-edge structure shows that the symmetry-breaking distorts the coordination environment and modulates the delocalized electrons around the Zn sites, which favors the formation of unpaired low-valence Znδ+ , thereby facilitating the adsorption/activation of N2 . Theoretical calculations elucidate that low-valence Znδ+ in Zn-N2 S2 -MOF can effectively lower the energy barrier of potential determining step, promoting the kinetics and boosting the NRR activity. This work highlights the relationship between the precise coordination environment of metal sites and the catalytic activity, which offers insightful guidance for rationally designing high-efficiency electrocatalysts.

Encapsulation of H4SiW12O40 into an Amide-Functionalized MOF: A Highly Efficient Nanocomposite Catalyst for Oxidative Desulfurization of Diesel Fuel.

Production of hydrocarbon fuels containing sulfur in ultralow levels is in high demand and requires the development of novel catalytic systems for oxidative desulfurization (ODS). Herein, a new nanocomposite SiW12@ZSTU-10 catalyst containing H4SiW12O40 (SiW12) encapsulated into a zinc(II) 3D metal-organic framework (MOF) (ZSTU-10) was assembled and characterized. The intricate structure and porosity of ZSTU-10 permit efficient encapsulation of the catalytically active SiW12 cages. The impact of different experimental parameters on the ODS of model oil containing dibenzothiophene as a typical S-based contaminant was evaluated. The SiW12@ZSTU-10 catalyst exhibits remarkable activity with up to 99.8% sulfur removal in 30 min. Kinetic features, trapping tests, and mechanistic studies were also performed. Furthermore, the catalyst offered an outstanding thermal and chemical stability, without apparent leaching and decline in the activity after six cycles. Such an improved catalytic efficiency of SiW12@ZSTU-10 can be assigned to (i) size-matched occupation of the ZSTU-10 pores by SiW12-active species, (ii) prevention of polyoxometalate (POM) leaching from the MOF matrix, (iii) facilitation of the access of S-based substrates to the active sites of SiW12, and (iv) excellent stability and recyclability of the obtained nanocomposite. The preset work widens a family of promising nanocomposite catalysts for improving the desulfurization performance of hybrid POM-MOF catalytic systems.

A macroporous carbon nanoframe for hosting Mott-Schottky Fe-Co/Mo2C sites as an outstanding bi-functional oxygen electrocatalyst.

Simultaneously optimizing the d-band center of the catalyst and the mass/charge transport processes during the oxygen catalytic reaction is an essential but arduous task in the pursuit of creating effective and long-lasting bifunctional oxygen catalysts. In this study, a Fe-Co/Mo2C@N-doped carbon macroporous nanoframe was successfully synthesized via a facile "conformal coating and coordination capture" pyrolysis strategy. As expected, the resulting heterogeneous electrocatalyst exhibited excellent reversible oxygen electrocatalytic performance in an alkaline medium, as demonstrated by the small potential gap of 0.635 V between the operating potential of 1.507 V at 10 mA cm-2 for the oxygen evolution reaction and the half-wave potential of 0.872 V towards the oxygen reduction reaction. Additionally, the developed Zn-air battery employing the macroporous nanoframe heterostructure displayed an impressive peak power density of 218 mW cm-2, a noteworthy specific capacity of 694 mA h gZn-1, and remarkable charging/discharging cycle durability. Theoretical calculations confirmed that the built-in electric field between the Fe-Co alloy and Mo2C semiconductor could induce advantageous charge transport and redistribution at the heterointerface, contributing to the optimization of the d-band center of the nanohybrid and ultimately leading to a reduction in the reaction energy barrier during catalytic processes. The exquisite macroporous nanoframe facilitated the rapid transport of ions and charges, as well as the smooth access of oxygen to the internal active site. Thus, the presented unique electronic structure regulation and macroporous structure design show promising potential for the development of robust bifunctional oxygen electrodes.

Efficient degradation of formaldehyde based on DFT-screened metal-doped C3N6 monolayer photocatalysts: performance evaluation and mechanistic insights.

Photocatalytic oxidation is an efficient and promising technology for reducing indoor pollution levels of formaldehyde (HCHO). However, developing efficient and low-cost photocatalysts for the removal of HCHO remains challenging due to the time-consuming and expensive nature of traditional "trial and error" and "directed research" approaches. To achieve this goal, first-principles density functional theory (DFT) calculations were conducted to high-throughput screen candidate TM-C3N6 photocatalysts for high-performance degradation of HCHO. The results revealed that Zr-C3N6 and Hf-C3N6 in functionalizing C3N6 with 28 transition metals showed excellent adsorption energy of HCHO, boosting the highly effective capture of HCHO. Meanwhile, an excellent adsorption performance mechanism was further elicited by the electric structure-property relationship. In addition, reaction mechanisms for HCHO degradation and three potential reaction pathways for HCHO degradation were systematically evaluated. Our findings indicated that hydroxyl-assisted dehydrogenation and oxygen-assisted dehydrogenation are the most favorable pathways, with rate-limiting steps involving the formation of ˙OH and ˙O radicals. Overall, this study may provide new insights into a high-throughput screening of novel photocatalysts that are both high-performing and low-cost for the removal of formaldehyde. This, in turn, can accelerate the experimental development process and reduce the associated costs and time consumption.

Dipole field in nitrogen-enriched carbon nitride with external forces to boost the artificial photosynthesis of hydrogen peroxide.

Artificial photosynthesis is a promising strategy for efficient hydrogen peroxide production, but the poor directional charge transfer from bulk to active sites restricts the overall photocatalytic efficiency. To address this, a new process of dipole field-driven spontaneous polarization in nitrogen-rich triazole-based carbon nitride (C3N5) to harness photogenerated charge kinetics for hydrogen peroxide production is constructed. Here, C3N5 achieves a hydrogen peroxide photosynthesis rate of 3809.5 µmol g-1 h-1 and a 2e- transfer selectivity of 92% under simulated sunlight and ultrasonic forces. This high performance is attributed to the introduction of rich nitrogen active sites of the triazole ring in C3N5, which brings a dipole field. This dipole field induces a spontaneous polarization field to accelerate a rapid directional electron transfer process to nitrogen active sites and therefore induces Pauling-type adsorption of oxygen through an indirect 2e- transfer pathway to form hydrogen peroxide. This innovative concept using a dipole field to harness the migration and transport of photogenerated carriers provides a new route to improve photosynthesis efficiency via structural engineering.