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Halogen substitution effect, as one of the most feasible chemical strategies for exploiting new ferroelectric materials, holds a promise to optimize spontaneous polarization ( P s ) and improve potential phase transition energy barrier. However, it is challenging to rationally regulate the photoferroelectric properties, e.g., ferroelectric photovoltaics. Through the p- site halogen substitution of spacer cations, we have obtained a series of two-dimensional hybrid perovskite ferroelectrics, (4 x -benzylammonium) 2 (ethylammonium) 2 Pb 3 Br 10 ((4 x -BA) 2 (EA) 2 Pb 3 Br 10 , abbreviated as 4 x -BEB, x  = F/Cl/Br/I), featuring the typical trilayered perovskite architecture. The p -site halogen-substituted BA + cations enable precise tuning of both the distortion degree of inorganic layer and the electric dipole moment of aromatic spacer. This molecular engineering not only drives a progressive enhancement of P s but also facilitates Br - ion migration, which are the driving forces for the ferroelectric anomalous photovoltaic effect (APVE). The member 4I-BEB shows a giant APVE of 38.2 V, exceeding other inorganic oxides and representing the highest value within the family of hybrid semiconductors. This halogen substitution strategy of spacer cations provides an effective way to design APV-active ferroelectric materials. The regulation of ferroelectric photovoltaic properties has been challenging. Here, authors substitute the p-site of cations with halogen for tuning distortion degree of inorganic layer and electric dipole moment of aromatic spacer, achieving ferroelectric anomalous photovoltaic effect of 38.2 V.

The light-induced pyroelectric effect (LPE) has shown a great promise in the application of optoelectronic devices, especially for self-powered detection and imaging. However, it is quite challenging and scarce to achieve LPE in the X-ray region. For the first time, we report X-ray LPE in a single-phase ferroelectric of (NPA)2(EA)2Pb3Br10 (1, NPA = neopentylamine, EA = ethylamine), adopting a two-dimensional trilayered perovskite motif, which has a large spontaneous polarization of ∼3.7 μC/cm2. Its ferroelectricity allows for significant LPE in the wavelength range of ordinary visible light. Strikingly, the X-ray LPE is observed in 1, which endows remarkable self-powered X-ray responses at 0 bias, including sensitivity up to 225 μC Gy–1 cm–2 and a low detection limit of ∼83.4 nGy s–1, being almost 66 times lower than the requirement for medical diagnostics (∼5.5 μGy s–1). This work not only develops a new mode for X-ray detection but also provides valuable insights for future photoelectric device application.

To modulate nonlinear optical (NLO) effects of crystalline material holds great application potential in the photoelectronic and optical fields. Organic configurationally‐locked polyene represents an exciting NLO family with large second harmonic generation (SHG) effects, whereas it is a huge blank to switch and modulate their NLO property through external stimuli. For the first time, here present unusual thermo‐enhanced SHG activities are presented in a polyene‐based NLO compound, 2‐3‐[2‐(4‐pyrrolidinphenyl)vinyl]‐5,5‐dimethylcyclohex‐2‐enylidenemalononitrile (1), giving a record‐high magnitude of SHG enhancement up to ≈170% during its isomorphic phase transition. Theoretical analysis discloses this behavior stems from the reduced degree of torsion in the π‐conjugated structures in 1, as verified by dihedral angles between its pyrrolidine and phenyl planes. As the first study on thermo‐enhanced SHG properties of organic crystals, this work affords a new avenue of modulating physical properties to fabricate high‐performance photoelectronic and optical devices. The unprecedented thermo‐enhanced second harmonic generation (SHG) response is achieved in an organic configurationally‐locked polyene nonlinear optical (NLO) crystal, ascribed to the decrease of torsion degree of the π‐conjugated bridge induced by the molecular dynamic motions. This work paves a new pathway to develop smart photoelectronics devices.

Heterostructure single crystals have emerged as a significant functional material system due to their unique properties and potential for novel optoelectronic device applications. Particularly, their distinctive structural characteristics offer promising prospects for suppressing ion migration, which is highly advantageous for X‐ray detection. Herein, by gradually modifying the cyclohexylmethylamine cation into the 4‐aminomethyltetrahydropyran cation, a layered heterostructure single crystal (PbCl2)2(4‐Aminomethyltetrahydropyran)2PbCl4 is successfully obtained. It comprises two distinct inorganic frameworks, namely a perovskite layer built from PbCl₆ octahedra and an intergrowth layer consisting of PbCl₂ units, wherein the organic components are firmly anchored to the intergrowth layer via Pb─O bonds, thereby enhancing the crystal stability and effectively suppressing ion migration, as evidenced by high ion migration activation energy (1.64 eV) and extremely low dark current drift (2.86 × 10−18 A cm−1 V−1 s−1). X‐ray devices based on the ultra‐stable heterostructure single crystal demonstrate an extraordinary sensitivity of 8453.3 µC Gy−1 cm−2 (at 40 V), ultra‐low detection limit of 5.2 nGy s−1 and superior air stability (≈1 year). Such values make it one of the most outstanding candidates for high‐performance X‐ray detection. This work promotes the development of heterostructure single crystals optoelectronic applications. This work reports a 2D heterostructure single crystal composed of two distinct inorganic frameworks, of which the ion migration is effectively inhibited by the strong interaction between organic components and inorganic layers. Such merits enable highly sensitive ultra‐stable X‐ray detection performances and highlight the potential of heterostructure single crystals for X‐ray applications.

Constraining the electrochemical reactivity of free solvent molecules is pivotal for developing high-voltage lithium metal batteries, especially for ether solvents with high Li metal compatibility but low oxidation stability ( <4.0 V vs Li + /Li). The typical high concentration electrolyte approach relies on nearly saturated Li + coordination to ether molecules, which is confronted with severe side reactions under high voltages ( >4.4 V) and extensive exothermic reactions between Li metal and reactive anions. Herein, we propose a molecular anchoring approach to restrict the interfacial reactivity of free ether solvents in diluted electrolytes. The hydrogen-bonding interactions from the anchoring solvent effectively suppress excessive ether side reactions and enhances the stability of nickel rich cathodes at 4.7 V, despite the extremely low Li + /ether molar ratio (1:9) and the absence of typical anion-derived interphase. Furthermore, the exothermic processes under thermal abuse conditions are mitigated due to the reduced reactivity of anions, which effectively postpones the battery thermal runaway. Advanced electrolyte is essential for high-energy-density lithium metal batteries. Here, the authors design a molecular anchoring dilute electrolyte via intermolecular hydrogen bonding with free solvents to improve the battery electrochemical and thermal stabilities.

Uncontrollable zinc (Zn) plating and hydrogen evolution greatly undermine Zn anode reversibility. Previous electrolyte designs focus on suppressing H 2 O reactivity, however, the accumulation of alkaline byproducts during battery calendar aging and cycling still deteriorates the battery performance. Here, we present a direct strategy to tackle such problems using a strong Brønsted acid, bis(trifluoromethanesulfonyl)imide (HTFSI), as the electrolyte additive. This approach reformulates battery interfacial chemistry on both electrodes, suppresses continuous corrosion reactions and promotes uniform Zn deposition. The enrichment of hydrophobic TFSI – anions at the Zn|electrolyte interface creates an H 2 O-deficient micro-environment, thus inhibiting Zn corrosion reactions and inducing a ZnS-rich interphase. This highly acidic electrolyte demonstrates high Zn plating/stripping Coulombic efficiency up to 99.7% at 1 mA cm –2 ( > 99.8% under higher current density and areal capacity). Additionally, Zn | |ZnV 6 O 9 full cells exhibit a high capacity retention of 76.8% after 2000 cycles. Trace amounts of strong acid can suppress Zn corrosion and promote uniform Zn deposition. Here, the authors use HTFSI to create a hydrophobic micro-environment at the Zn-electrolyte interface, enabling high efficiency and cycling stability.

Rechargeable aqueous zinc batteries (RAZBs) offer a promising solution for large-scale energy storage due to the abundance, low cost, and safety of Zn. However, practical applications are hindered by Zn anode instability, dendrite growth, and hydrogen evolution reactions (HER). Chaotropic Zn(ClO 4 ) 2 electrolytes are favorable for low-temperature operations but exacerbate these issues due to their high acidity, leading to severe Zn corrosion and layered double hydroxide formation. We propose a biomimetic strategy using methylguanidoacetic acid (creatine) as a low-cost, eco-friendly additive to address these challenges. Creatine acts as a proton pocket to finely tune the pH of acidic Zn(ClO 4 ) 2 electrolytes for suppressing HER and stabilizing the Zn anode. Furthermore, the formed creatinine cations adsorb on the Zn surface, promoting highly controlled Zn deposition with a preferred (002) orientation. This approach significantly enhances battery cycling performance, with Zn∥Zn cells demonstrating extended cycling stability at both low and high current densities. Zn∥Cu cells exhibited improved Coulombic efficiency over thousands of cycles, indicating highly reversible Zn plating/stripping. Notably, stable cell operations were realized at the temperature as low as −35°C without electrolyte freezing. Our findings highlight the potential of biomimetic proton regulation and interfacial modulation for improving the stability and reversibility of Zn plating/stripping in RAZBs.

Background Inflammatory bowel disease (IBD) involves a breakdown in interactions between the host immune response and the resident commensal microbiota. Recent studies have suggested gut physiology and pathology relevant to human IBD can be rapidly modeled in zebrafish larvae. The aim of this study was to investigate the dysbiosis of intestinal microbiota in zebrafish models with IBD-like enterocolitis using culture-independent techniques. Results IBD-like enterocolitis was induced by exposing larval zebrafish to trinitrobenzenesulfonic acid (TNBS). Pathology was assessed by histology and immunofluorescence. Changes in intestinal microbiota were evaluated by denaturing gradient gel electrophoresis (DGGE) and the predominant bacterial composition was determined with DNA sequencing and BLAST and confirmed by real-time polymerase chain reaction. Larval zebrafish exposed to TNBS displayed intestinal-fold architecture disruption and inflammation reminiscent of human IBD. In this study, we defined a reduced biodiversity of gut bacterial community in TNBS-induced coliitis. The intestinal microbiota dysbiosis in zebrafish larvae with IBD-like colitis was characterized by an increased proportion of Proteobacteria (especially Burkholderia ) and a decreased of Firmicutes( Lactobacillus group ), which were significantly correlated with enterocolitis severity(Pearson correlation p < 0.01). Conclusions This is the first description of intestinal microbiota dysbiosis in zebrafish IBD-like models, and these changes correlate with TNBS-induced enterocolitis. Prevention or reversal of this dysbiosis may be a viable option for reducing the incidence and severity of human IBD.

摘要 目的 比较消渴通痹方(XF)与普瑞巴林治疗痛性糖尿病神经病变(PDN)的疗效和安全性。 方法 对68例PDN患者进行单中心, 随机, 单盲, 双模拟, 平行对照临床试验。主要结果是糖尿病周围神经病变的简明疼痛问卷(BPI‐DPN)的变化。次要结果包括BPI‐DPN下降>50%, 疼痛数字评定量表‐11(NRS‐11)评分的变化, 日常睡眠干预日记(DSID), 患者总体变化印象(PGIC), 神经传导速度(NCV)和不良事件。 结果 治疗10周后, XF组和普瑞巴林组的BPI‐DPN评分分别从42.44±17.56降至26.47±22.22和52.03±14.30降至37.85±17.23(P<0.001)。两组间BPI‐DPN评分绝对值变化差异为‐1.79(95%CI:‐9.09, 5.50, P=0.625)。XF组和普瑞巴林组分别有44.1%(15/34)和20.6%(7/34)的患者报告BPI‐DPN下降>50%(P=0.038)。两组间NRS‐11和DSID评分差异无统计学意义(P>0.05)。与普瑞巴林组相比, XF组有显著改善或改善的患者数量显著增加(35.3%(12/34)比11.8%(4/34), P=0.045)。两组右侧正中神经运动传导速度绝对值变化差异有统计学意义(XF组0.70±2.3vs.普瑞巴林组‐2.2±4.1, P=0.004)。两组均未报告严重不良事件。 结论 XF在减轻PDN患者疼痛症状, 提高生活质量方面与普瑞巴林相当。此外, XF还有可能通过增加神经传导速度来改善神经功能。