Latest ArticlesFinding suitable strategies to effectively enhance the optical properties of materials are the goal being pursued by researchers. Herein, cation-anion synergetic interactions strategy was proposed to develop two novel organic-inorganic hybrid antimony-based optical materials, (C3H5N2)SbF2SO4 (Ⅰ) and (C5H6N)SbF2SO4 (Ⅱ), which were obtained by introducing Sb3+cation containing stereochemically active lone-pair (SCALP) and organic π-conjugated cations into sulphate system. The synergistic interactions of the organic π-conjugated cations, the inorganic [SbO2F2]3− seesaw anions and the [SO4]2− distorted tetrahedra anions make their ultraviolet (UV) absorption edges approach 297 and 283 nm, respectively, and raise their birefringence up to 0.193@546 nm and 0.179@546 nm, respectively. Interestingly, although the two compounds have the same stoichiometric ratio and similar one-dimensional (1D) chain structure, they show opposite macroscopic symmetry, where the NCS compound (Ⅱ) exhibits a large second-harmonic generation (SHG) response (1.6 times that of KH2PO4). The two reported compounds are found to be promising UV optical materials in the experimental tests.
Catalysts can significantly promote the reaction dynamics and are therefore considered crucial components for achieving high electrochemical energy conversion efficiency. However, the active sites of the catalysts, particularly for nano-level and atomic-level catalysts commonly undergo reconstruction under practical applications. Therefore, obtaining an in-depth and systematic understanding on the real active sites through in situ/operando characterization techniques is a prerequisite for establishing the structure-performance relationship and guiding the future design of more efficient electrocatalysts. Herein, we summarize the recent progress of in situ/operando characterization techniques for identifying the nature of active sites of electrocatalysts when used in electrocatalytic energy conversion reaction. Specifically, our focus lies in the fundamental principles of various in situ/operando characterization techniques, with particular emphasis on their applications for electrocatalytic reactions. Beyond that, the challenges and perspective insights are also added in the final section to highlight the future direction of this important field.
In order to advance the commercialization of rechargeable Li-air batteries, it is of importance to explore cathode catalyst with efficient catalytic activity. Transition metal oxides have poor electrical conductivity, while cobalt phosphide has excellent electrical conductivity and large specific surface area. Nevertheless, its application in organic Li-air batteries has been much less studied, and the electrocatalytic activity desires to be further elevated. Here, CoP/Co2P heterojunction composite with higher polarity was fabricated. The discharge product of high-polarity CoP/Co2P had a new porous box-like morphology, which was easy to be decomposed and exposed more active sites. The highly polar CoP/Co2P heterostructure composite had homogeneous pores, the synergistic effect existed between CoP and Co2P, and the discharge product was porous box mixed with Li2O2 and LiOH, which made CoP/Co2P achieve high specific capacity of 14632 mAh/g and cycle stably 161 times when used as air electrode cathode catalyst. This work furnished a thought for the construction of cathode catalysts with efficient catalytic activity for Li-air batteries.
Electrocatalytic water splitting is the most directly available route to generate renewable and sustainable hydrogen. Here, we report the design of a composite material in which arrays of square pillar-like NiMoO4 nanorods coated with N, P-doped carbon layers are uniformly contained in numerous nested nanoparticle structures. The catalysts have superior catalytic activity, requiring only 59 mV and 187 mV for HER and OER to attain a current density of 10 mA/cm2, respectively. The assembled two-electrode electrolytic cell required a voltage of 1.48 V to reach 10 mA/cm2, along with excellent long-term stability. Theoretical calculations reveal that electrons aggregate and redistribute at the heterogeneous interface, with the d-band centers of the Ni and Fe atoms being positively shifted compared to the Fermi level, effectively optimizing the adsorption of intermediates and reducing the Gibbs free energy, thus accelerating the catalytic process. Meanwhile, an integrated solar-driven water-splitting system demonstrated a high and stable solar-to-hydrogen efficiency of 18.20%. This work provides new possibilities for developing non-precious metal-based bifunctional electrocatalysts for large-scale water splitting applications.
Strategic active site organization is imperative for the advancement of effective and long-lasting catalysts of oxygen reduction reactions. However, the controllable multi-active site design is a highly intricate topic for catalyst synthesis. Employing pre-trapping and post-activation strategy, Fe-N bonding structure and S, Se functionalized heteroatom are integrated into a conductive porous carbon. In this process, the nitrogen-abundant polymer 1,3,5-triformylbenzene-tris(4-aminophenyl)benzene (Tf-TAPA) adsorbs Fe3+ under the intrinsically metal anchoring ability of N atoms and simultaneously in-situ assembles long-chain thiophene-S. Subsequently, the Fe3+ is transformed into Fe-Nx moieties with the conversion of the organic chain to incompletely graphitized carbon. Furthermore, the alteration of the electronic configuration achieved through the introduction of dual-atom S and Se leads to a pronounced enhancement in catalytic efficiency. Benefitting from the Fe-Nx bonding structure, dense structural defects, and conductive carbon networks, the resultant Fe-S,Se/NCNs possesses a positive half-wave potential of 0.86 V and a 90% current retention rate, outstripping the Pt/C benchmark. Moreover, the liquid and flexible ZAB driven by Fe-S,Se/NCNs achieves large power densities of 259.7 and 164.7 mW/cm2, respectively. This study provides a new comprehension in developing an efficient and stable M-N-C oxygen electrocatalyst.
X-ray detection plays a crucial role across various aspects of our daily lives, encompassing medical diagnoses, security screenings, and non-destructive examinations in industrial settings. Given the wide array of application contexts, a wealth of opportunities is entailed with the practical utilization of both organic and inorganic X-ray detection materials. A novel and promising contender in this realm is the emergence of metal-free organic halide perovskites (O-PVSKs), offering great opportunities and tremendous potential in X-ray detection. This potential can be attributed to the distinct crystalline configuration of O-PVSKs, where organic constituents are structured into an ABX3 perovskite arrangement. Consequently, O-PVSKs exhibit captivating characteristics reminiscent of organic materials, such as lightweight nature and modifiability, all while retaining the distinctive traits associated with halide perovskites ranging from diverse structures to tunable optoelectronic properties. This review article delves into the intrinsic attributes of O-PVSKs and critically examines the viability of O-PVSKs in X-ray detection, through which key features that distinguish O-PVSKs from traditional organic semiconductors and perovskites are outlined. This is followed by a perspective given on their future avenues for exploration.
To solve the volume expansion and poor electrical conductivity of germanium-based anode materials, Ge/rGO/CNTs nanocomposites with three-dimensional network structure are fabricated through the dispersion of polyethylene-polypropylene glycol (F127) and reduction of hydrogen. An interesting phenomenon is discovered that F127 can break GeO2 polycrystalline microparticles into 100 nm nanoparticles by only physical interaction, which promotes the uniform dispersion of GeO2 in a carbon network structure composed of graphene (rGO) and carbon nanotubes (CNTs). As evaluated as anode material of Lithium-ion batteries, Ge/rGO/CNTs nanocomposites exhibit excellent lithium storage performance. The initial specific capacity is high to 1549.7 mAh/g at 0.2 A/g, and the reversible capacity still retains 972.4 mAh/g after 100 cycles. The improved lithium storage performance is attributed to that Ge nanoparticles can effectively slow down the volume expansion during charge and discharge processes, and three-dimensional carbon networks can improve electrical conductivity and accelerate lithium-ion transfer of anode materials.
With the increasing demand for high energy density energy storage device, Li metal has received intensive attention for its ultrahigh capacity and the lowest redox potential. LiNO3 is widely used as electrolyte additive for ether electrolyte, which can improve the cycle performance of Li metal anode. Compared to ethers, carbonates are more suitable for Li metal batteries with high voltage cathode because they have a wider electrochemical window. However, LiNO3 performs poor solubility in carbonate electrolyte, restricting its application in high voltage Li battery. Herein, we presented a facile method to introduce abundant LiNO3 additive to carbonate electrolyte system by introducing LiNO3-PAN es as the interlayer of the cell. LiNO3-PAN es is in sufficient contact with the electrolyte so that it can continuously releases LiNO3 to assist the formation of Li2N2O2-rich single nitrogenous component SEI layer on Li surface. With the help of LiNO3-PAN es, Li metal anode shows excellent cycle stability even at a high current density of 4 mA/cm2, so that the cycle performance of the full cells was significantly improved, whether in the anode-free Cu||LFP cell or the Li||NCM622 cell.
Carbon monoxide (CO) is a vital intracellular gas messenger known for its cytoprotective and homeostatic properties. It plays a pivotal role in a myriad of biological processes. Therefore, the precise detection of CO is of paramount importance in unraveling the intricacies of pathological mechanisms and advancing the development of disease diagnosis. We herein introduce NFCOP, a state-of-the-art near-infrared (NIR) turn-on fluorescence (FL) probe that has been meticulously designed for highly sensitive, swift and selective imaging of CO. The NFCOP response occurred rapidly with CO, within just 10 s, and the calculated detection limit for CO was determined to be 0.32 µmol/L. Further investigations conducted at the cellular level and in vivo demonstrated that NFCOP possesses high sensitivity and selectivity for imaging CO.
Theranostic carbon dots (CDs) have attracted widespread attention recently due to their tunable optical properties and diverse bioactivities. Beyond fluorescent imaging application, the photothermal property endows CDs with the potential for microbial inactivation. However, realization of the effective conversion between fluorescence and heat in one CD system has rarely been reported. Herein, we provide a simple strategy for targeted microbial theranostics based on 4-carboxyphenylboronic acid-derived CDs (PCBA-CDs) which possess concentration-dependent photoluminescence/photothermal features. At lower concentrations, PCBA-CDs show bright and stable fluorescent signals ranging from blue to green. The fluorescence intensity gradually decreases with increasing concentration, while on the contrary, the photothermal effect of PCBA-CDs ascends progressively due to the rearrangement of electronic transitions in aggregated CDs. PCBA-CDs also demonstrate high affinity to the polysaccharide structures on the surface of microbe which allows rapid microbial fluorescence imaging as well as specific photothermal ablation of pathogens in skin wounds using PCBA-CDs at lower and higher concentrations, respectively. This study supplies a facile nanotheranostic strategy for just-in-time microbial management using bioactive CDs.
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