Latest ArticlesLithium (Li)–CO2 battery is rising as an attractive energy-storage system with the competence of CO2 conversion/fixation. However, its practical development is seriously hindered by the high overpotential. Herein, a rational design on a highly catalytic Li–CO2 battery electrode built by graphdiyne powder as a multi-functional laminar scaffold with anchored highly dispersed Ru nanoparticles is explored. The strong interaction between the abundant acetylenic bond sites of graphdiyne scaffold and Ru nanoparticles can effectively promote the electrochemical progress and reduce the voltage polarization. The unique channels architecture of the cathodic catalyst with enough space not only accelerates CO2 diffusion and electrons/Li+ transport, but also allows a large amount of accommodation for discharged product (Li2CO3) to assure an advanced capacity. The corresponding Li–CO2 battery displays an advanced discharged capacity of 15,030 mAh/g at 500 mA/g, great capacity retention of 8873 mAh/g at 2 A/g, high coulombic efficiency of 97.6% at 500 mA/g and superior life span for 120 cycles with voltage gap of 1.67 V under a restricted capacity of 1000 mAh/g at 500 mA/g. Ex/in-situ studies prove that synergy between Ru nanoparticles and acetylene bonds of GDY can boost the round-trip CO2RR and CO2ER kinetics.
NH3 in ambient air directly leads to an increase in the aerosol content in the air. These substances lead to the formation of haze to various environmental problems after atmospheric circulation and diffusion. Controlling NH3 emissions caused by ammonia escaping from mobile and industrial sources can effectively reduce the NH3 content in ambient air. Among the various NH3 removal methods, the selective catalytic oxygen method (NH3-SCO) is committed to oxidizing NH3 to environmentally harmless H2O and N2; therefore, it is the most valuable and ideal ammonia removal method. In this review, the characteristics of loaded and core-shell catalysts in NH3-SCO have been reviewed in the context of catalyst structure-activity relationships, and the H2O resistance and SO2 resistance of the catalysts are discussed in the context of practical application conditions. Then the effects of the valence state of the active center, oxygen species on the catalyst surface, dispersion of the active center and acidic sites on the catalyst performance are discussed comprehensively. Finally, the shortcomings of the existing catalysts are summarized and the catalyst development is discussed based on the existing studies.
Carbon aerogels prepared from renewable nano building blocks are rising-star materials and hold great promise in many fields. However, various defects formed during carbonization at high temperature disfavor the stress transfer and thus the fabrication of flexible carbon aerogel from renewable nano building blocks. Herein, a structural defect-reducing strategy is proposed by altering the pyrolysis route of cellulose nanofiber. Inorganic salt that inhibits the generation of tar volatilization during pyrolysis can prevent the formation of various structural defects. Microstructure with fewer defects can reduce stress concentration and remarkably enhance the compressibility of carbon aerogel, thus increasing the maximum stress retention of carbon aerogel. The carbon aerogel also has high stress sensor sensitivity and excellent temperature coefficient of resistance. The structural defect-reducing strategy will pave a new way to fabricate high-strength carbon materials for various fields.
A dimesitylboryl-ended oligothiophene with tetrazine as core (BTz) was synthesized and its reactivity and spectral changes toward trans-cyclooctene ((4E)-TCO-OH), cis-cyclooctene and bicyclo[6.1.0]non-4-yn-9-ylmethanol were comprehensively studied. The fluorescence intensity of BTz was enhanced up to more than 100 times upon bioorthogonal reaction with (4E)-TCO-OH. In addition, the first crystal structure of isolated product of tetrazine derivative with cyclooctene was determined, which clearly confirmed a dehydrogenation occurred after Diels–Alder reaction under ambient conditions.
Aqueous zinc-ion batteries (AZIBs) have become a hotspot for electrochemical energy storage owing to the high safety, low cost, environmental friendliness, and favorable rate performance. However, the serious dissolution of cathode materials in aqueous electrolytes would lead to poor cyclability, which should be addressed before commercialization. Herein, we designed a Ti-doped V2O5 with yolk-shell microspherical structure for AZIBs. The Ti doping stabilizes the crystal structure and relieves the dissolution of V2O5 in aqueous ZnSO4 electrolyte. The optimized sample, Ti0.2V1.8O4.9, delivers a high capacity (355 mAh/g at 0.05 A/g) as well as good capacity retention (89% after 2500 cycles at 1.0 A/g). This work provides an effective strategy to mitigate the dissolution of cathode material in aqueous ZnSO4 electrolyte for cyclability enhancement.
A method for the generation of alkyl radicals from inert alkyl C-O bonds has been developed via an iron/borane reagent/alkoxide catalytic system, which can be employed for the synthesis of amines from nitroarenes with excellent efficiency. Preliminary mechanistic studies reveal that the amine synthesis may be involving a single electron transfer pathway to form alkyl radicals, and the low-valent iron species may be the active intermediates.
We have synthesized two copper nanoclusters (NCs) with a protection of the same ligand diphenylphosphino-2-pyridine (C17H14NP, dppy for short), formulated as Cu4(dppy)4Cl2 and Cu21(dppy)10, respectively. The former one bears a distorted tetrahedron Cu4 core with its six edges fully protected by chlorine and dppy ligands, while the latter presents a symmetric Cu21 core on which ten dppy molecules function as monolayer protection via well-organized monodentate or bidentate coordination. Interestingly, the Cu4(dppy)4Cl2 cluster exhibits a strong yellow emission at ~577 nm, while Cu21(dppy)10 displays dual emissions in purple (~368 nm) and green (~516 nm) regions respectively. In combination with TD-DFT calculations, we demonstrate the origin of altered emissions and unique stability of the two copper nanoclusters pertaining to the ligand coordination and metallic superatomic states.
Carbon dots (CDs) have attracted considerable attention as a new type of fluorescent carbon nanomaterial because of their excellent optical properties, biocompatibility, and high electrical conductivity. Research on CDs has been conducted for nearly two decades and has focused on numerous precursors, various synthesis conditions and properties and applications of CDs. Biomass is critical in the green development of CDs because of its low cost, environmental friendliness, and sustainable properties. This review focuses on the advantages and applications of biomass-derived CDs. In addition, the challenges of photobleaching, toxicity, and stability of biomass-based CDs are discussed in detail. Lastly, the prospects and challenges of biomass-derived CDs are highlighted.
The A2A adenosine receptor (A2AAR) has attracted attention as an emerging immunotherapeutic target with several antagonists being evaluated in clinical trials. However, A2AAR antagonists show limited efficacy as monotherapies. Herein, we communicate our design and synthesis of a novel series of A2AAR/histone deacetylase (HDAC) bifunctional inhibitors, based on the core structure of the A2AAR antagonist PBF-509. The new compounds were designed using a pharmacophore-merging strategy and features a tri-substituted pyrimidine core. The binding affinity for A2AAR and inhibitory activity against HDACs of all the new compounds were tested. A number of compounds exhibited nanomolar or subnanomolar activity against both targets and some showed equally potent antiproliferative activity against MC38, CT26 and HCT116 colon cancer lines compared to HDAC inhibitors SAHA and MGCD-0103 in vitro. The binding poses of compound 5a in both A2AAR and HDAC1 were predicted by molecular docking studies. Collectively, these results suggest these tri-substituted pyrimidine derivatives are promising leads for developing A2AAR/HDAC dual-acting compounds as novel antitumor agents.
Photodynamic therapy (PDT) is a clinically approved cancer treatment that uses energy of light to generate active substances that cause damage to the cancer. Photosensitizers are employed to absorb light and generate toxic reactive oxygen species (ROS) to damage biomolecules like DNA. At the same time, some chemotherapy drugs like nucleotide analogues can provide mechanism-guided promotion in the treatment efficacy of PDT. However, the photosensitizer and chemotherapy drugs used in PDT is usually organic molecules, which suffers from bad solubility, fast clearance, and acute toxicity. To achieve targeted treatment, a reasonable delivery system is necessary. Therefore, we reported a metal-phenolic network where IR780 and gemcitabine were coupled chemically to overcome these shortcomings. The enhanced PDT effects can be realized by the promoted cell death both in vitro and in vivo. Moreover, the synergistic therapy also induced T-cell mediated anti-tumor immune response, which was significant for the inhibition of distant tumor growth. This work expanded the biomedical application of metal-phenolic materials and contribute to the wider application of photodynamic cancer therapy.
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