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.     

Challenges and Opportunities of Implantable Neural Interfaces: From Material,Electrochemical and Biological Perspectives

The desirable implantable neural interfaces can accurately record bioelectrical signals from neurons and regulate neural activities with high spatial/time resolution, facilitating the understanding of neuronal functions and dynamics. However, the electrochemical performance (impedance, charge storage/injection capacity) is limited with the miniaturization and integration of neural electrodes. The “crosstalk” caused by the uneven distribution of elctric field leads to lower electrical stimulation/recording efficiency. The mismatch between stiff electrodes and soft tissues exacerbates the inflammatory responses, thus weakening the transmission of signals. Though remarkable breakthroughs have been made through the incorporation of optimizing electrode design and functionalized nanomaterials, the chronic stability, and long-term activity in vivo of the neural electrodes still need further development. In this review, the neural interface challenges mainly on electrochemistry and biology are discussed, followed by summarizing typical electrode optimization technologies and exploring recent advances in the application of nanomaterials, based on traditional metallic materials, emerging 2D materials, conducting polymer hydrogels, etc., for enhancing neural interfaces. The strategies for improving the durability including enhanced adhesion and minimized inflammatory response, are also summarized. The promising directions are finally presented to provide enlightenment for high-performance neural interfaces in future, which will promote profound progress in neuroscience research.     

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.     

基于用户行为的社交网络人格特质识别方法

社交网络已成为人们获取和发布信息的一个重要平台,也是黑客发起网络诈骗的主要场地。大多数黑客在发起网络诈骗之前,首先会判别目标用户的主要人格特点,然后根据主要人格特点制定与其接触的策略。因此,面向社交网络用户的人格特质识别方法的研究对提高用户识别社交网络诈骗能力具有重要意义。提出基于用户的人格特质识别方法。通过构建面向社交网络的人格特质词典提取用户发表或转发文本信息中能反映用户主要人格特质类型的观测值,采用5个具有不同参数值的隐半马尔可夫模型刻画用户在社交网络上发表或转发文本信息的行为过程。在人格特质识别阶段,通过计算每个用户在发表或转发文本信息过程中产生的观测序列相对于模型的平均对数似然概率,以识别用户所属的人格特质类型。在采集的新浪微博数据集上进行实验,结果表明,当假正率为10%时,该方法的总真正率为93.18%,能准确识别用户的人格特质类型。     

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.     

Hydrofluoric Acid-Removable Additive Optimizing Electrode Electrolyte Interphases with Li+ Conductive Moieties for 4.5 V Lithium Metal Batteries

High-voltage lithium metal batteries (LMBs) are capable to achieve the increasing energy density. However, their cycling life is seriously affected by unstable electrolyte/electrode interfaces and capacity instability at high voltage. Herein, a hydrofluoric acid (HF)-removable additive is proposed to optimize electrode electrolyte interphases for addressing the above issues. N, N-dimethyl-4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl) aniline (DMPATMB) is used as the electrolyte additive to induce PF₆⁻ decomposition to form a dense and robust LiF-rich solid electrolyte interphase (SEI) for suppressing Li dendrite growth. Moreover, DMPATMB can help to form highly Li⁺ conductive Li₃N and LiBO₂, which can boost the Li⁺ transport across SEI and cathode electrolyte interphase (CEI). In addition, DMPATMB can scavenge traced HF in the electrolyte to protect both SEI and CEI from the corrosion. As expected, 4.5 V Li|| LiNi_0.6Co_0.2Mn_0.2O₂ batteries with such electrolyte deliver 145 mAh g⁻¹ after 140 cycles at 200 mA g⁻¹. This work provides a novel insight into high-voltage electrolyte additives for LMBs.     

Grafted MXenes Based Electrolytes for 5V-Class Solid-State Batteries

Polymer blends based solid polymer electrolytes (SPEs), combining the advantages of multiple polymers, are promising for the utilization of 5 V-class cathodes (e.g., LiCoMnO₄ (LCMO)) with enhanced safety. However, severe macro-phase separation with defects and voids in polymer blends restrict the electrochemical stability and ionic migration of SPEs. Herein, inorganic compatibilizer polyacrylonitrile grafted MXene (MXene-g-PAN) is exploited to improve the miscibility of the poly(vinylidene fluoride-co-hexafluoropropylene) (PVHF)/PAN blends and suppress the consolidation of phase particles. The resulting SPE exhibits a high anodic stability with an ionic conductivity of 2.17 × 10⁻⁴ S cm⁻¹, enabling a stable and reversible Li platting/stripping (over 2500 h). The fabricated solid Li‖LCMO cell delivers a 5.1 V discharge voltage with a decent capacity (131 mAh g⁻¹) and cycling performance. Subsequently, the solid all-in-one graphite‖LCMO battery is also constructed to extend the application of MXene based SPEs in flexible batteries. Benefiting from the interface-less design, outstanding mechanical flexibility and stability is achieved in the battery, which can endure various deformations with a low-capacity loss (< ≈10%). This study signifies a significant development on solid flexible lithium ion batteries with enhanced performance, stability, and reliability by investigating the miscibility of polymer blends, benefiting for the design of high-performance SPEs.     

High-Performing Quasi-2D Perovskite Photodetectors with Efficient Charge Transport Network Built from Vertically Orientated and Evenly Distributed 3D-Like Phases

Quasi-two-dimensional (Q-2D) perovskites are emerging as one of the most promising materials for photodetectors. However, a significant challenge to Q-2D perovskites for photodetection is their insufficient charge transport ability, which is mainly attributed to their hybrid low-dimensional n-phase structure. This study demonstrates that evenly-distributed 3D-like phases with vertical orientation throughout the film can greatly facilitate charge transport and suppress charge recombination, outperforming the prevalent phase structure with a vertical dimension gradient. Based on such a phase structure, a Q-2D Ruddlesden−Popper perovskite self-powered photodetector achieving a combination of exceptional figures-of-merit is realized, including a responsivity of 0.45 AW⁻¹, a peak specific detectivity of 2.3 × 10¹³ Jones, a 156 dB linear dynamic range, and a rise/fall time of 2.89 µs/1.93 µs. The desired phase structure is obtained by utilizing a double-hole transport layer (HTL), combining hydrophobic PTAA and hydrophilic PEDOT: PSS. Besides, the dependence of the hybrid low-dimensional phase structure is also identified on the surface energy of the buried HTL substrate. This study gives insight into the correlation between Q-2D perovskites’ phase structure and performance, providing a valuable design guide for Q-2D perovskite-based photodetectors.     

A Polymer Defect Passivator for Efficient Hole-Conductor-Free Printable Mesoscopic Perovskite Solar Cells

Due to the low cost and excellent potential for mass production, printable mesoscopic perovskite solar cells (p-MPSCs) have drawn a lot of attention among other device structures. However, the low open-circuit voltage (V_OC) of such devices restricts their power conversion efficiency (PCE). This limitation is brought by the high defect density at perovskite grain boundaries in the mesoporous scaffold, which results in severe nonradiative recombination and is detrimental to the V_OC. To improve the perovskite crystallization process, passivate the perovskite defects, and enhance the PCE, additive engineering is an effective way. Herein, a polymeric Lewis base polysuccinimide (PSI) is added to the perovskite precursor solution as an additive. It improves the perovskite crystallinity and its carbonyl groups strongly coordinate with Pb²⁺, which can effectively passivate defects. Additionally, compared with its monomer, succinimide (SI), PSI serves as a better defect passivator because the long-chained macromolecule can be firmly anchored on those defect sites and form a stronger interaction with perovskite grains. As a result, the champion device has a PCE of 18.84%, and the V_OC rises from 973 to 1030 mV. This study offers a new strategy for fabricating efficient p-MPSCs.     

Catalytically Induced Robust Inorganic-Rich Cathode Electrolyte Interphase for 4.5 V Li||NCM622 Batteries

Tailoring inorganic components of cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI) is critical to improving the cycling performance of lithium metal batteries. However, it is challenging due to complicated electrolyte reactions on cathode/anode surfaces. Herein, the species and inorganic component content of the CEI/SEI is enriched with an objectively gradient distribution through employing pentafluorophenyl 4-nitrobenzenesulfonate (PFBNBS) as electrolyte additive guided by engineering bond order with functional groups. In addition, a catalytic effect of LiNi_0.6Mn_0.2Co_0.2O₂ (NCM622) cathode is proposed on the decomposition of PFBNBS. PFBNBS with lower highest occupied molecular orbital can be preferentially oxidized on the NCM622 surface with the help of the catalytic effect to induce an inorganic-rich CEI for superior electrochemical performance at high voltage. Moreover, PFBNBS can be reduced on the Li surface due to its lower lowest unoccupied molecular orbital , increasing inorganic moieties in SEI for inhibiting Li dendrite generation. Thus, 4.5 V Li||NCM622 batteries with such electrolyte can retain 70.4% of initial capacity after 500 cycles at 0.2 C, which is attributed to the protective effect of the excellent CEI on NCM622 and the inhibitory effect of its derived CEI/SEI on continuous electrolyte decomposition.