Carbon Black-Supported Single-Atom Co?N?C as an Efficient Oxygen Reduction Electrocatalyst for H2O2 Production in Acidic Media and Microbial Fuel Cell in Neutral Media

Single metal atom isolated in nitrogen-doped carbon materials (M N C) are effective electrocatalysts for oxygen reduction reaction (ORR), which produces H₂O₂ or H₂O via 2-electron or 4-electron process. However, most of M N C catalysts can only present high selectivity for one product, and the selectivity is usually regulated by complicated structure design. Herein, a carbon black-supported Co N C catalyst (CB@Co N C) is synthesized. Tunable 2-electron/4-electron behavior is realized on CB@Co-N-C by utilizing its H₂O₂ yield dependence on electrolyte pH and catalyst loading. In acidic media with low catalyst loading, CB@Co N C presents excellent mass activity and high selectivity for H₂O₂ production. In flow cell with gas diffusion electrode, a H₂O₂ production rate of 5.04 mol h⁻¹ g⁻¹ is achieved by CB@Co N C on electrolyte circulation mode, and a long-term H₂O₂ production of 200 h is demonstrated on electrolyte non-circulation mode. Meanwhile, CB@Co N C exhibits a dominant 4-electron ORR pathway with high activity and durability in pH neutral media with high catalyst loading. The microbial fuel cell using CB@Co N C as the cathode catalyst shows a peak power density close to that of benchmark Pt/C catalyst.     

Solution-Mediated Hybrid FAPbI3 Perovskite Quantum Dots for Over 15% Efficient Solar Cell

Organic–inorganic formamidinium lead triiodide (FAPbI₃) hybrid perovskite quantum dot (QD) is of great interest to photovoltaic (PV) community due to its narrow band gap, higher ambient stability, and long carrier lifetime. However, the surface ligand management of FAPbI₃ QD is still a key hurdle that impedes the design of high-efficiency solar cells. Herein, this study first develops a solution-mediated ligand exchange (SMLE) for preparing FAPbI₃ QD film with enhanced electronic coupling. By dissolving optimal methylammonium iodide (MAI) into antisolvent to treat the FAPbI₃ QD solution, the SMLE can not only effectively replace the long-chain ligands, but also passivate the A- and X-site vacancies. By combining experimental and theoretical results, this study demonstrates that the SMLE engineered FAPbI₃ QD exhibits lower defect density, which is beneficial for fabricating high-quality QD arrays with desired morphology and carrier transport. Consequently, the SMLE FAPbI₃ QD based solar cell outputs a champion efficiency of 15.10% together with improved long-term ambient storage stability, which is currently the highest reported value for hybrid perovskite QD solar cells. These results would provide new design principle of hybrid perovskite QDs toward high-performance optoelectronic application.     

Ultraefficient Non-Doped Deep Blue Fluorescent OLED: Achieving a High EQE of 10.17% at 1000 cd m−2 with CIEy<0.08

The pursuit for efficient deep blue material is an ever-increasing issue in organic optoelectronics field. It is a long-standing challenge to achieve high external quantum efficiency (EQE) exceed 10% at brightness of 1000 cd m⁻² with a Commission International de L'Eclairage (CIE_y) <0.08 in non-doped organic light-emitting diodes (OLEDs). Herein, this study reports a deep blue luminogen, PPITPh, by bonding phenanthro[9,10-d]imidazole moiety with m-terphenyl group via benzene bridge. The non-doped OLED based on PPITPh exhibits an exceptionally high EQE of 11.83% with a CIE coordinate of (0.15, 0.07). The EQE still maintains 10.17% at the brightness of 1000 cd m⁻², and even at a brightness as high as 10000 cd m⁻², an EQE of 7.5% is still remained, representing the record-high result among non-doped deep-blue OLEDs at 1000 cd m⁻². The unprecedented device performance is attributed to the reversed intersystem crossing process through hot exciton mechanism. Besides, the maximum EQE of orange phosphorescent OLED with PPITPh as host is 32.02%, and remains 31.17% at the brightness of 1000 cd m⁻². Such minimal efficiency roll-off demonstrates that PPITPh is also an excellent phosphorescent host material. The result offers a new design strategy for the enrichment of high-efficiency deep blue luminogen.     

Ni3N–CeO2 Heterostructure Bifunctional Catalysts for Electrochemical Water Splitting

Developing low-cost and high-efficient bifunctional catalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is greatly significant for water electrolysis. Here, Ni₃N-CeO₂/NF heterostructure is synthesized on the nickel foam, and it exhibits excellent HER and OER performance. As a result, the water electrolyzer based on Ni₃N-CeO₂/NF bifunctional catalyst only needs 1.515 V@10 mA cm⁻², significantly better than that of Pt/C||IrO₂ catalysts. In situ characterizations unveil that CeO₂ plays completely different roles in HER and OER processes. In situ infrared spectroscopy and density functional theory calculations indicate that the introduction of CeO₂ can optimizes the structure of interface water, and the synergistic effect of Ni₃N and CeO₂ improve the HER activity significantly, while the in situ Raman spectra reveal that CeO₂ accelerates the reconstruction of O_V (oxygen vacancy)-rich NiOOH for boosting OER. This study clearly unlocks the different catalytic mechanisms of CeO₂ for boosting the HER and OER activity of Ni₃N for water splitting, which provides the useful guidance for designing the high-performance bifunctional catalysts for water splitting.     

Reduced Graphene Oxides Modified Bi2Te3 Nanosheets for Rapid Photo-Thermoelectric Catalytic Therapy of Bacteria-Infected Wounds

Temperature variation-induced thermoelectric catalytic efficiency of thermoelectric material is simultaneously restricted by its electrical conductivity, Seebeck coefficient, and thermal conductivity. Herein, Bi₂Te₃ nanosheets are in situ grown on reduced graphene oxides (rGO) to generate an efficient photo-thermoelectric catalyst (rGO-Bi₂Te₃). This system exhibits phonon scattering effect and extra carrier transport channels induced by the formed heterointerface between rGO and Bi₂Te₃, which improves the power factor value and reduces thermal conductivity, thus enhancing the thermoelectric performance of 2.13 times than single Bi₂Te₃. The photo-thermoelectric catalysis of rGO-Bi₂Te₃ significantly improves the reactive oxygen species yields, resulting from the effective electron–hole separation caused by the unique thermoelectric field and heterointerfaces of rGO-Bi₂Te₃. Correspondingly, the electrospinning membranes containing rGO-Bi₂Te₃ nanosheets exhibit high antibacterial efficiency in vivo (99.35 ± 0.29%), accelerated tissue repair ability, and excellent biosafety. This study provides an insight into heterointerface design in photo-thermoelectric catalysis.     

A NIR-II AIEgen-Based Supramolecular Nanodot for Peroxynitrite-Potentiated Mild-Temperature Photothermal Therapy of Hepatocellular Carcinoma

Compared to conventional photothermal therapy (PTT) which requires hyperthermia higher than 50 °C, mild-temperature PTT is a more promising antitumor strategy with much lower phototoxicity to neighboring normal tissues. However, the therapeutic efficacy of mild-temperature PTT is always restricted by the thermoresistance of cancer cells. To address this issue, a supramolecular drug nanocarrier is fabricated to co-deliver nitric oxide (NO) and photothermal agent DCTBT with NIR-II aggregation-induced emission (AIE) characteristic for mild-temperature PTT. NO can be effectively released from the nanocarriers in intracellular reductive environment and DCTBT is capable of simultaneously producing reactive oxygen species (ROS) and hyperthermia upon 808 nm laser irradiation. The generated ROS can further react with NO to produce peroxynitrite (ONOOˉ) bearing strong oxidization and nitration capability. ONOOˉ can inhibit the expression of heat shock proteins (HSP) to reduce the thermoresistance of cancer cells, which is necessary to achieve excellent therapeutic efficacy of DCTBT-based PTT at mild temperature (<50 °C). The antitumor performance of ONOOˉ-potentiated mild-temperature PTT is validated on subcutaneous and orthotopic hepatocellular carcinoma (HCC) models. This research puts forward an innovative strategy to overcome thermoresistance for mild-temperature PTT, which provides new inspirations to explore ONOOˉ-sensitized tumor therapy strategies.