Abstract: The oxidation of hydrocarbons to produce high value-added compounds (ketones or alcohols) using oxygen in air as the only oxidant is an efficient synthetic strategy from both environmental and economic views. Herein, we successfully synthesized cobalt single atom site catalysts (Co SACs) with high metal loading of 23.58 wt.% supported on carbon nitride (CN), which showed excellent catalytic properties for oxidation of ethylbenzene in air. Moreover, Co SACs show a much higher turn-over frequency (19.6 h−1) than other reported non-noble catalysts under the same condition. Comparatively, the as-obtained nanosized or homogenous Co catalysts are inert to this reaction. Co SACs also exhibit high selectivity (97%) and stability (unchanged after five runs) in this reaction. DFT calculations reveal that Co SACs show a low energy barrier in the first elementary step and a high resistance to water, which result in the robust catalytic performance for this reaction.

Abstract: There is an emerging need for high-sensitivity solar-blind deep ultraviolet (DUV) photodetectors with an ultra-fast response speed. Although nanoscale devices based on Ga2O3 nanostructures have been developed, their practical applications are greatly limited by their slow response speed as well as low specific detectivity. Here, the successful fabrication of two-/three-dimensional (2D/3D) graphene (Gr)/PtSe2/β-Ga2O3 Schottky junction devices for high-sensitivity solar-blind DUV photodetectors is demonstrated. Benefitting from the high-quality 2D/3D Schottky junction, the vertically stacked structure, and the superior-quality transparent graphene electrode for effective carrier collection, the photodetector is highly sensitive to DUV light illumination and achieves a high responsivity of 76.2 mA/W, a large on/off current ratio of ~ 105, along with an ultra-high ultraviolet (UV)/visible rejection ratio of 1.8 × 104. More importantly, it has an ultra-fast response time of 12 µs and a remarkable specific detectivity of ~ 1013 Jones. Finally, an excellent DUV imaging capability has been identified based on the Gr/PtSe2/β-Ga2O3 Schottky junction photodetector, demonstrating its great potential application in DUV imaging systems.

Abstract: An effective electrocatalyst being highly active in all pH range for oxygen reduction reaction (ORR) is crucial for energy conversion and storage devices. However, most of the high-efficiency ORR catalysis was reported in alkaline conditions. Herein, we demonstrated the preparation of atomically dispersed Fe-Zn pairs anchored on porous N-doped carbon frameworks (Fe-Zn-SA/NC), which works efficiently as ORR catalyst in the whole pH range. It achieves high half-wave potentials of 0.78, 0.85 and 0.72 V in 0.1 M HClO4, 0.1 M KOH and 0.1 M phosphate buffer saline (PBS) solutions, respectively, as well as respectable stability. The performances are even comparable to Pt/C. Furthermore, when assembled into a Zn-air battery, the high power density of 167.2 mWcm−2 and 120 h durability reveal the feasibility of Fe-Zn-SA/NC in real energy-related devices. Theoretical calculations demonstrate that the superior catalytic activity of Fe-Zn-SA/NC can be contributed to the lower energy barriers of ORR at the Fe-Zn-N6 centers. This work demonstrates the potential of Fe-Zn pairs as alternatives to the Pt catalysts for efficient catalytic ORR and provides new insights of dual-atom catalysts for other energy conversion related catalytic reactions.

Abstract: Perovskite variants have attracted wide interest because of the lead-free nature and strong self-trapped exciton (STE) emission. Divalent Sn(II) in CsSnX3 perovskites is easily oxidized to tetravalent Sn(IV), and the resulted Cs2SnCl6 vacancy-ordered perovskite variant exhibits poor photoluminescence property although it has a direct band gap. Controllable doping is an effective strategy to regulate the optical properties of Cs2SnX6. Herein, combining the first principles calculation and spectral analysis, we attempted to understand the luminescence mechanism of Te4+-doped Cs2SnCl6 lead-free perovskite variants. The chemical potential and defect formation energy are calculated to confirm theoretically the feasible substitutability of tetravalent Te4+ ions in Cs2SnCl6 lattices for the Sn-site. Through analysis of the absorption, emission/excitation, and time-resolved photoluminescence (PL) spectroscopy, the intense green-yellow emission in Te4+:Cs2SnCl6 was considered to originate from the triplet Te(IV) ion 3P1→1S0 STE recombination. Temperature-dependent PL spectra demonstrated the strong electron-phonon coupling that inducing an evident lattice distortion to produce STEs. We further calculated the electronic band structure and molecular orbital levels to reveal the underlying photophysical process. These results will shed light on the doping modulated luminescence properties in stable lead-free Cs2MX6 vacancy-ordered perovskite variants and be helpful to understand the optical properties and physical processes of doped perovskite variants.

Abstract: Nanozymes are nanomaterials with enzyme-like properties that have attracted significant interest owing to their capability to address the limitations of traditional enzymes such as fragility, high cost, and impossible mass production. Over the past decade, a broad variety of nanomaterials have been found to mimic the enzyme-like activity by engineering the active centers of natural enzymes or developing multivalent elements within nanostructures. Carbon nanomaterials with well-defined electronic and geometric structures have served as favorable surrogates of traditional enzymes by mimicking the highly evolved catalytic center of natural enzymes. In particular, by combining the unique electronic, optical, thermal, and mechanical properties, carbon nanomaterials-based nanozymes can offer a variety of multifunctional platforms for biomedical applications. In this review, we will introduce the enzymatic characteristics and recent advances of carbon nanozymes, and summarize their significant applications in biomedicine.

Abstract: Photocatalytic production of hydrogen peroxide (H2O2) is an ideal pathway for obtaining solar fuels. Herein, an S-scheme heterojunction is constructed in hybrid TiO2/In2S3 photocatalyst, which greatly promotes the separation of photogenerated carriers to foster efficient H2O2 evolution. These composite photocatalysts show a high H2O2 yield of 376 µmol/(L·h). The mechanism of charge transfer and separation within the S-scheme heterojunction is well studied by computational methods and experiments. Density functional theory and in-situ irradiated X-ray photoelectron spectroscopy results reveal distinct features of the S-scheme heterojunction in the TiO2/In2S3 hybrids and demonstrate charge transfer mechanisms. The density functional theory calculation and electron paramagnetic resonance results suggest that O2 reduction to H2O2 follows stepwise one-electron processes. In2S3 shows a much stronger interaction with O2 than TiO2 as well as a higher reduction ability, serving as the active sites for H2O2 generation. The work provides a novel design of S-scheme photocatalyst with high H2O2 evolution efficiency and mechanistically demonstrates the improved separation of charge carriers.

Abstract: Development of efficient non-precious catalysts for seawater electrolysis is of great significance but challenging due to the sluggish kinetics of oxygen evolution reaction (OER) and the impairment of chlorine electrochemistry at anode. Herein, we report a heterostructure of Ni3S2 nanoarray with secondary Fe-Ni(OH)2 lamellar edges that exposes abundant active sites towards seawater oxidation. The resultant Fe-Ni(OH)2/Ni3S2 nanoarray works directly as a free-standing anodic electrode in alkaline artificial seawater. It only requires an overpotential of 269 mV to afford a current density of 10 mA·cm−2 and the Tafel slope is as low as 46 mV·dec−1. The 27-hour chronopotentiometry operated at high current density of 100 mA·cm−2 shows negligible deterioration, suggesting good stability of the Fe·Ni(OH)2/Ni3S2@NF electrode. Faraday efficiency for oxygen evolution is up to ∼ 95%, revealing decent selectivity of the catalyst in saline water. Such desirable catalytic performance could be benefitted from the introduction of Fe activator and the heterostructure that offers massive active and selective sites. The density functional theory (DFT) calculations indicate that the OER has lower theoretical overpotential than Cl2 evolution reaction in Fe sites, which is contrary to that of Ni sites. The experimental and theoretical study provides a strong support for the rational design of high-performance Fe-based electrodes for industrial seawater electrolysis.

Abstract: Electrochemical nitrogen reduction reaction (NRR) is considered as an alternative to the industrial Haber-Bosch process for NH3 production due to both low energy consumption and environment friendliness. However, the major problem of electrochemical NRR is the unsatisfied efficiency and selectivity of electrocatalyst. As one group of the cheapest and most abundant transition metals, iron-group (Fe, Co, Ni and Cu) electrocatalysts show promising potential on cost and performance advantages as ideal substitute for traditional noble-metal catalysts. In this minireview, we summarize recent advances of iron-group-based materials (including their oxides, hydroxides, nitrides, sulfides and phosphides, etc.) as non-noble metal electrocatalysts towards ambient N2-to-NH3 conversion in aqueous media. Strategies to boost NRR performances and perspectives for future developments are discussed to provide guidance for the field of NRR studies.

Abstract: Strain sensors with good stability are vital to the development of wearable healthcare monitoring systems. However, the design of strain sensor with both duration stability and environmental stability is still a challenge. In this work, we propose an ultra-stable and washable strain sensor by embedding a coupled composite film of carbon nanotube (CNT) and Ti3C2Tx MXene into polydimethylsiloxane (PDMS) matrix. The composite strain sensor with embedded microstructure and uneven surface makes it conformal to skin, while the CNT/MXene sensing layer exhibits a resistance sensitive to strain. This sensor shows reliable responses at different frequencies and with long-term cycling durability (over 1,000 cycles). Meanwhile, the CNT/MXene/PDMS composite strain sensor provides the advantages of superior anti-interference to temperature change and water washing. The results demonstrate less than 10% resistance changes as the temperature rises from −20 to 80 °C or after sonication in water for 120 min, respectively. The composite sensor is applied to monitor human joint motions, such as bending of finger, wrist and elbow. Moreover, the simultaneous monitoring of the electrocardiogram (ECG) signal and joint movement while riding a sports bicycle is demonstrated, enabling the great potential of the as-fabricated sensor in real-time human healthcare monitoring.

Abstract: Two-dimensional (2D) van der Waals transition metal dichalcogenides (TMDs) are a new class of electronic materials offering tremendous opportunities for advanced technologies and fundamental studies. Similar to conventional semiconductors, substitutional doping is key to tailoring their electronic properties and enabling their device applications. Here, we review recent progress in doping methods and understanding of doping effects in group 6 TMDs (MX2, M = Mo, W; X = S, Se, Te), which are the most widely studied model 2D semiconductor system. Experimental and theoretical studies have shown that a number of different elements can substitute either M or X atoms in these materials and act as n- or p-type dopants. This review will survey the impact of substitutional doping on the electrical and optical properties of these materials, discuss open questions, and provide an outlook for further studies.

Abstract: Graphene is a material with unique properties that can be exploited in electronics, catalysis, energy, and bio-related fields Although, for maximal utilization of this material, high-quality graphene is required at both the growth process and after transfer of the graphene film to the application-compatible substrate Chemical vapor deposition (CVD) is an important method for growing high-quality graphene on non-technological substrates (as, metal substrates, eg, copper foil) Thus, there are also considerable efforts toward the efficient and non-damaging transfer of quality of graphene on to technologically relevant materials and systems In this review article, a range of graphene current transfer techniques are reviewed from the standpoint of their impact on contamination control and structural integrity preservation of the as-produced graphene In addition, their scalability, cost- and time-effectiveness are discussed We summarize with a perspective on the transfer challenges, alternative options and future developments toward graphene technology

Abstract: Metal-nitrogen-carbon (M-N-C) single-atom catalysts exhibit desirable electrochemical catalytic properties. However, the replacement of N atoms by heteroatoms (B, P, S, etc.) has been regarded as a useful method for regulating the coordination environment. The structure engineered M-N-C sites via doping heteroatoms play an important role to the adsorption and activation of the oxygen intermediate. Herein, we develop an efficient strategy to construct dual atomic site catalysts via the formation of a Co1-PN and Ni1-PN planar configuration. The developed Co1-PNC/Ni1-PNC catalyst exhibits excellent bifunctional electrocatalytic performance in alkaline solution. Both experimental and theoretical results demonstrated that the N/P coordinated Co/Ni sites moderately reduced the binding interaction of oxygen intermediates. The Co1-PNC/Ni1-PNC endows a rechargeable Zn-air battery with excellent power density and cycling stability as an air-cathode, which is superior to that of the benchmark Pt/C+IrO2. This work paves an avenue for design of dual single-atomic sites and regulation of the atomic configuration on carbon-based materials to achieve high-performance electrocatalysts.

Abstract: Electrochemical CO2 reduction reaction (CO2RR) is an attractive pathway for closing the anthropogenic carbon cycle and storing intermittent renewable energy by converting CO2 to valuable chemicals and fuels. The production of highly reduced carbon compounds beyond CO and formate, such as hydrocarbon and oxygenate products with higher energy density, is particularly desirable for practical applications. However, the productivity towards highly reduced chemicals is typically limited by high overpotential and poor selectivity due to the multiple electron-proton transfer steps. Tandem catalysis, which is extensively utilized by nature for producing biological macromolecules with multiple enzymes via coupled reaction steps, represents a promising strategy for enhancing the CO2RR performance. Improving the efficiency of CO2RR via tandem catalysis has recently emerged as an exciting research frontier and achieved significant advances. Here we describe the general principles and also considerations for designing tandem catalysis for CO2RR. Recent advances in constructing tandem catalysts, mainly including bimetallic alloy nanostructures, bimetallic heterostructures, bimetallic core-shell nanostructures, bimetallic mixture catalysts, metal-metal organic framework (MOF) and metal-metallic complexes, metal-nonmetal hybrid nanomaterials and copper-free hybrid nanomaterials for boosting the CO2RR performance are systematically summarized. The study of tandem catalysis for CO2RR is still at the early stage, and future research challenges and opportunities are also discussed.

Abstract: The hydrogen evolution reaction (HER) of molybdenum disulfide (MoS2) is limited in alkaline and acid solution because the active sites are on the finite edge with extended basal plane remaining inert. Herein, we activated the interfacial S sites by coupling with Ru nanoparticles on the inert basal plane of MoS2 nanosheets. The density functional theory (DFT) calculation and experimental results show that the interfacial S electronic structure was modulated. And the results of ΔGH* demonstrate that the adsorption of H on the MoS2 was also optimized. With the advantage of interfacial S sites activation, the Ru-MoS2 needs only overpotential of 110 and 98 mV to achieve 10 mA·cm−2 in both 0.5 M H2SO4 and 1 M KOH solution, respectively. This strategy paves a new way for activating the basal plane of other transition metal sulfide electrocatalysts for improving the HER performance.

Abstract: Oxygen evolution reaction (OER) is the key step involved both in water splitting devices and rechargeable metal-air batteries, and hence, there is an urgent need for a stable and low-cost material for efficient OER. In the present investigation, Co−Fe−Ga−Ni−Zn (CFGNZ) high entropy alloy (HEA) has been utilized as a low-cost electrocatalyst for OER. Herein, after cyclic voltammetry activation, CFGNZ-nanoparticles (NPs) are covered with oxidized surface and form high entropy (oxy) hydroxides (HEOs), exhibiting a low overpotential of 370 mV to achieve a current density of 10 mA/cm2 with a small Tafel slope of 71 mV/dec. CFGNZ alloy has higher electrochemical stability in comparison to state-of-the art RuO2 electrocatalyst as no degradation has been observed up to 10 h of chronoamperometry. Transmission electron microscopy (TEM) studies after 10 h of long-term chronoamperometry test showed no change in the crystal structure, which confirmed the high stability of CFGNZ. The density functional theory (DFT) based calculations show that the closeness of d(p)-band centers to the Fermi level (EF) plays a major role in determining active sites. This work highlights the tremendous potential of CFGNZ HEA for OER, which is the primary reaction involved in water splitting.

Abstract: Carbon dots (CDs) have attracted much attention due to their excellent photoelectric properties and potential applications. Although previous studies have shown that almost all organic molecules can be converted into CDs via chemical carbonization, the mechanism of the conversion process remains unclear. The hydrothermal/solvothermal method commonly used to prepare CDs is complicated and leads to the generation of many by-product CDs with similar structures. Considering that the purification of the synthesized by-products is difficult, the process of CDs formation cannot be readily analyzed and understood. Herein, we use ethanol as a carbon source to synthesize white-emitting CDs (W-CDs). Column chromatography separation shows that the synthesized W-CDs are composed of blue-, cyan-, and yellow-emitting CDs that fluoresce at wavelengths corresponding to the three emission centers of W-CDs. Although the samples have similar graphitic structure, they exhibit different surface states due to variations in the degree of oxidation and carbonization. Therefore, the red-shift in their emission peaks is attributed to an increased degree of carbonization in their polymer structure. Theoretical calculations verify the experimental results, and the prepared CDs are successfully used to develop multi-color and white light-emitting diodes (LEDs).

Abstract: The construction and design of highly efficient and inexpensive bifunctional oxygen electrocatalysts substitute for noble-metal-based catalysts is highly desirable for the development of rechargeable Zn-air battery (ZAB). In this work, a bifunctional oxygen electrocatalysts of based on ultrafine CoFe alloy (4-5 nm) dispersed in defects enriched hollow porous Co-N-doped carbons, made by annealing SiO2 coated zeolitic imidazolate framework-67 (ZIF-67) encapsulated Fe ions. The hollow porous structure not only exposed the active sites inside ZIF-67, but also provided efficient charge and mass transfer. The strong synergetic coupling among high-density CoFe alloys and Co-Nx sites in Co, N-doped carbon species ensures high oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activity. First-principles simulations reveal that the synergistic promotion effect between CoFe alloy and Co-N site effectively reduced the formation energy of from O* to OH*. The optimized CoFe-Co@PNC exhibits outstanding electrocatalytic stability and activity with the overpotential of only 320 mV for OER at 10 mA·cm−2 and the half-wave potential of 0.887 V for ORR, outperforming that of most recent reported bifunctional electrocatalysts. A rechargeable ZAB constructed with CoFe-Co@PNC as the air cathode displays long-term cyclability for over 200 h and high power density (152.8 mW·cm−2). Flexible solid-state ZAB with our CoFe-Co@PNC as the air cathode possesses a high open circuit potential (OCP) up to 1.46 V as well as good bending flexibility. This universal structure design provides an attractive and instructive model for the application of nanomaterials derived from MOF in the field of sustainable flexible energy applications device.

Abstract: Oxygen vacancy (Vo) is important in the modification of electrode for rechargeable batteries. However, due to the scarcity of suitable preparation strategy with controllable Vo incorporation, the impact of Vo concentration on the electrochemical performances remains unclear. Thus, in this work, Vo-V2O5-PEDOT (VoVP) with tunable Vo concentration is achieved via a spontaneous polymerization strategy, with the capability of mass-production. The introduction of poly(2,3-dihydrothieno-1,4-dioxin) (PEDOT) not only leads to the formation of Vo in V2O5, but it also results in a larger interlayer spacing. The as-prepared Vo-V2O5-PEDOT-20.3% with Vo concentration of 20.3% (denoted as VoVP-20) is able to exhibit high capacity of 449 mAh·g−1 at current density of 0.2 A·g−1, with excellent cyclic performance of 94.3% after 6,000 cycles. It is shown in the theoretical calculations that excessive Vo in V2O5 will lead to an increase in the band gap, which inhibits the electrochemical kinetics and charge conductivity. This is further demonstrated in the experimental results as the electrochemical performance starts to decline when Vo concentration increases beyond 20.3%. Thus, based on this work, scalable fabrication of high-performance electrode with tunable Vo concentration can be achieved with the proposed strategy.

Abstract: Industrial-scale ammonia (NH3) production mainly relies on the energy-intensive and environmentally unfriendly Haber-Bosch process. Such issue can be avoided by electrocatalytic N2 reduction which however suffers from limited current efficiency and NH3 yield. Herein, we demonstrate ambient NH3 production via electrochemical nitrite (NO2−) reduction catalyzed by a CoP nanoarray on titanium mesh (CoP NA/TM). When tested in 0.1 M PBS (pH = 7) containing 500 ppm NO2−, such CoP NA/TM is capable of affording a large NH3 yield of 2,260.7 ± 51.5 µg·h−1·cm−2 and a high Faradaic efficiency of 90.0 ± 2.3% at −0.2 V vs. a reversible hydrogen electrode. Density functional theory calculations reveal that the potential-determining step for NO2− reduction over CoP (112) is *NO2 → *NO2H.

Abstract: Lithium metal (Li) is believed to be the ultimate anode for lithium-ion batteries (LIBs) owing to the advantages of high theoretical capacity, the lowest electrochemical potential, and light weight. Nevertheless, issues such as uncontrollable growth of Li dendrites, large volume changes, high chemical reactivity, and unstable solid electrolyte interphase (SEI) hinder its rapid development and practical application. Herein a stable and dendrite-free Li-metal anode is obtained by designing a flexible and freestanding MXene/COF framework for metallic Li. COF-LZU1 microspheres are distributed among the MXene film framework. Lithiophilic COF-LZU1 microspheres as nucleation seeds can promote uniform Li nucleation by homogenizing the Li+ flux and lowering the nucleation barrier, finally resulting in dense and dendrite-free Li deposition. Under the regulation of the COF-LZU1 seeds, the Coulombic efficiency of the MXene/COF-LZU1 framework and electrochemical stability of corresponding symmetric cells are obviously enhanced. Li-S full cells with the modified Li-metal anode and sulfurized polyacrylonitrile (S@PAN) cathode also exhibited a superior electrochemical performance.

Abstract: Molybdenum disulfide (MoS2) has been recognized as one of the most promising candidates to replace precious Pt for hydrogen evolution reaction (HER) catalysis, due to the natural abundance, low cost, tunable electronic properties, and excellent chemical stability. Although notable processes have been achieved in the past decades, their performance is still far less than that of Pt. Searching effective strategies to boosting their HER performance is still the primary goal. In this review, the recent process of the electronic regulation of MoS2 for HER is summarized, including band structure engineering, electronic state modulation, orbital orientation regulation, interface engineering. Last, the key challenges and opportunities in the development of MoS2-based materials for electrochemical HER are also discussed.

Abstract: Engineering of defects in semiconductors provides an effective protocol for improving photocatalytic N2 conversion efficiency. This review focuses on the state-of-the-art progress in defect engineering of photocatalysts for the N2 reduction toward ammonia. The basic principles and mechanisms of thermal catalyzed and photon-induced N2 reduction are first concisely recapped, including relevant properties of the N2 molecule, reaction pathways, and NH3 quantification methods. Subsequently, defect classification, synthesis strategies, and identification techniques are compendiously summarized. Advances of in situ characterization techniques for monitoring defect state during the N2 reduction process are also described. Especially, various surface defect strategies and their critical roles in improving the N2 photoreduction performance are highlighted, including surface vacancies (i.e., anionic vacancies and cationic vacancies), heteroatom doping (i.e., metal element doping and nonmetal element doping), and atomically defined surface sites. Finally, future opportunities and challenges as well as perspectives on further development of defect-engineered photocatalysts for the nitrogen reduction to ammonia are presented. It is expected that this review can provide a profound guidance for more specialized design of defect-engineered catalysts with high activity and stability for nitrogen photochemical fixation.

Abstract: The key challenge for scalable production of hydrogen from water lies in the rational design and preparation of high-performance and earth-abundant electrocatalysts to replace precious metal Pt and IrO2 for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Although atomic M-N-C materials have been extensively studied in heterogeneous catalysis field, the insufficient antioxidant capacity of carbonous substrates hinders their practical application in OER. Developing highly active and stable OER electrocatalysts is the key for electrochemical water splitting. This review presents feasible design strategies for fabricating carbon-free single-site catalysts and their applications in HER/OER and overall water splitting. The constitutive relationships between structure, composition, and catalytic performance for HER and OER are detailly discussed, providing ponderable insights into rationally constructing high-performance HER and OER electrocatalysts. The perspectives on the challenges and future research orientations in single-site catalysts for electrochemical water splitting are suggested.

Abstract: The next generation of electronics technology is purely going to be based on wearable sensing systems. Wearable electronic sensors that can operate in a continuous and sustainable manner without the need of an external power sources, are essential for portable and mobile electronic applications. In this review article, the recent progress and advantages of wearable self-powered smart chemical sensors systems for wearable electronics are presented. An overview of various modes of energy conversion and storage technologies for self-powered devices is provided. Self-powered chemical sensors (SPCS) systems with integrated energy units are then discussed, separated as solar cell-based SPCS, triboelectric nano-generators based SPCS, piezoelectric nano-generators based SPCS, energy storage device based SPCS, and thermal energy-based SPCS. Finally, the outlook on future prospects of wearable chemical sensors in self-powered sensing systems is addressed.

Abstract: Full-color emissive carbon dots (CDs) hold a great promise for various applications, especially in light emitting diodes (LEDs). However, the existing synthetic routes for CDs are carried out in solutions, which suffer from low yields, high pressures, various byproducts, large amounts of waste solvents, and complicated photoluminescence (PL) origins. Therefore, it is necessary to explore large scale synthesis of CDs with high quantum yield (QY) across the entire visible range from a single carbon source by a solvent-free method. In this work, a series of CDs with tunable PL emission from 442 to 621 nm, QY of 23%–56%, and production yield within 34%–72%, are obtained by heating o-phenylenediamine with the catalysis of KCl. Detailed characterizations identify that, the differences between these CDs with respect to the graphitization degree, graphitic nitrogen content, and oxygen-containing functional groups, are responsible for their distinct optical properties, which can be modulated by controlling the deamination and dehydrogenation processes during reactions. Blue, green, yellow, red emissive films, and LEDs are prepared by dispersing the corresponding CDs into polyvinyl alcohol (PVA). All types of white LEDs (WLEDs) with high colorrendering- index (CRI), including warm WLEDs, standard WLEDs, and cool WLEDs, are also fabricated by mixing the red, green, and blue emissive CDs into PVA matrix by the appropriate ratios.

Abstract: Metal sulfide based materials as photocatalysts for energy conversion are essential to produce value-added chemical fuels, but their intrinsically slow carrier dynamics and low activity are yet to be resolved. Herein, we developed a unique heterogeneously nanostructured ZnIn2S4-CdS heterostructure that involves zero-dimensional (0D) CdS quantum dots uniformly confined on three-dimensional (3D) ZnIn2S4 nanoflowers, which achieves an excellent catalytic performance of CO2 photoconversion under visible-light irradiation. The obtained hierarchical heterostructure can significantly enhance the light harvesting, shorten the migration distance of carriers, and obviously accelerate the transport of electrons. As evidenced by the ultrafast transient absorption spectroscopy, the formed interface can effectively facilitate charge separation and transport. This work opens up a new avenue to carefully design the elaborate heterostructures for achieving optimal charge separation efficiency by lowering interfacial kinetic barriers and energy losses at the interface.

Abstract: Electrochemical CO2 reduction reaction (CO2RR) offers a practical solution to current global greenhouse effect by converting excessive CO2 into value-added chemicals or fuels. Noble metal-based nanomaterials have been considered as efficient catalysts for the CO2RR owing to their high catalytic activity, long-term stability and superior selectivity to targeted products. On the other hand, they are usually loaded on different support materials in order to minimize their usage and maximize the utilization because of high price and limited reserve. The strong metal-support interaction (MSI) between the metal and substrate plays an important role in affecting the CO2RR performance. In this review, we mainly focus on different types of support materials (e.g., oxides, carbons, ligands, alloys and metal carbides) interacting with noble metal as electrocatalysts for CO2RR. Moreover, the positive effects about MSI for boosting the CO2RR performance via regulating the adsorption strength, electronic structure, coordination environment and binding energy are presented. Lastly, emerging challenges and future opportunities on noble metal electrocatalysts with strong MSI are discussed.

Abstract: Developing cost-effective, efficient and bifunctional electrocatalysts is vital for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) application. The catalytic activity of electrocatalysts could be optimized by reasonable electronic structure regulation and increasing active sites. Herein, we report the design and fabrication of Mo-doped nickel sulfide/hydroxide heterostructures (Mo-NiS/Ni(OH)2) as a multisite water splitting catalyst via straightforward solvothermal and in-situ growth strategy. Based on foreign metal doping and interface interaction, the electronic conductivity of heterostructures is improved and the charge transfer kinetics across the interface is promoted, which are demonstrated by the theoretical calculations. Mo-NiS/Ni(OH)2 electrocatalyst is endowed with high electrocatalytic performance for water splitting and remarkable durability in alkaline electrolyte. It exhibits the low overpotential of 186 and 74 mV at 10 mA·cm−2 for OER and HER, respectively. Importantly, after continuously working for 50 h, the current densities of HER and OER both show negligible degeneration. Even, the resulting Mo-NiS/Ni(OH)2 better catalyzes water splitting, yielding a current density of 10 mA·cm−2 at a cell voltage of 1.5 V and outperforming Pt/C-IrO2 couple (1.53 V). This result demonstrates that transition metal doping and heterogeneous interface engineering are useful means for conventional catalyst design.