In Situ Construction of Built-In Opposite Electric Field Balanced Surface Adsorption for Hydrogen Evolution Reaction.

Achieving a balance between H-atom adsorption and binding with H2 desorption is crucial for catalyzing hydrogen evolution reaction (HER). In this study, the feasibility of designing and implementing built-in opposite electric fields (OEF) is demonstrated to enable optimal H atom adsorption and H2 desorption using the Ni3(BO3)2/Ni5P4 heterostructure as an example. Through density functional theory calculations of planar averaged potentials, it shows that opposite combinations of inward and outward electric fields can be achieved at the interface of Ni3(BO3)2/Ni5P4, leading to the optimization of the H adsorption free energy (ΔGH*) near electric neutrality (0.05 eV). Based on this OEF concept, the study experimentally validated the Ni3(BO3)2/Ni5P4 system electrochemically forming Ni3(BO3)2 through cyclic voltammetry scanning of B-doped Ni5P4. The surface of Ni3(BO3)2 undergoes reconstruction, as characterized by Grazing Incidence Wide-Angle X-ray Scattering (GIWAXS) and in situ Raman spectroscopy. The resulting catalyst exhibits excellent HER activity in alkaline media, with a low overpotential of 33 mV at 10 mA cm-2 and stability maintained for over 360 h. Therefore, the design strategy of build-in opposite electric field enables the development of high-performance HER catalysts and presents a promising approach for electrocatalyst advancement.

Physical Mechanism and Chemical Trends in the Thermal Expansion of Inorganic Halide Perovskites.

The considerable thermal expansion of halide perovskites is one of the challenges to device stability, yet the physical origin and modulation strategy remain unclear. Herein, we report first-principles calculations of the thermal properties of halide perovskites at 300 K using oxides as a reference. We found that the large thermal expansion of halide perovskites can mainly be attributed to their low bulk modulus and volumetric heat capacity because of the soft crystal lattice, whereas composition-dependent anharmonicity emerges as the most important factor in determining thermal expansion with the same structure. We discovered that thermal expansion of halide perovskites can be decreased by weakening the B-X bond to promote the octahedral anharmonicity. We further proposed an effective thermal expansion coefficient descriptor of halide perovskites with a Pearson correlation coefficient of nearly -80%. Our findings provide insights into the underlying mechanisms and chemical trends in the thermal expansion behavior of halide perovskites.

Pressure-Tuning Photothermal Synergy to Optimize the Photoelectronic Properties in Amorphous Halide Perovskite Cs3 Bi2 I9.

Effective modification of the structure and properties of halide perovskites via the pressure engineering strategy has attracted enormous interest in the past decade. However, sufficient effort and insights regarding the potential properties and applications of the high-pressure amorphous phase are still lacking. Here, the superior and tunable photoelectric properties that occur in the pressure-induced amorphization process of the halide perovskite Cs3 Bi2 I9 are demonstrated. With increasing pressure, the photocurrent with xenon lamp illumination exhibits a rapid increase and achieves an almost five orders of magnitude increment compared to its initial value. Impressively, a broadband photoresponse from 520 to 1650 nm with an optimal responsivity of 6.81 mA W-1 and fast response times of 95/96 ms at 1650 nm is achieved upon successive compression. The high-gain, fast, broadband, and dramatically enhanced photoresponse properties of Cs3 Bi2 I9 are the result of comprehensive photoconductive and photothermoelectric mechanisms, which are associated with enhanced orbital coupling caused by an increase in BiI interactions in the [BiI6 ]3- cluster, even in the amorphous state. These findings provide new insights for further exploring the potential properties and applications of amorphous perovskites.

Pressure-Tailored Self-Driven and Broadband Photoresponse in PbI2.

Photoelectric devices based on the photothermoelectric (PTE) effect show promising prospects for broadband detection without an external power supply. However, effective strategies are still required to regulate the conversion efficiency of light to heat and electricity. Herein, significantly enhanced photoresponse properties of PbI2 generated from a PTE mechanism via a high-pressure strategy are reported. PbI2 exhibits a stable, fast, self-driven, and broadband photoresponse at ≈980 nm. Intriguingly, the synergy of the photoconductivity and PTE mechanism is conducive to enhancing the photoelectric properties, and extending the detection bandwidth to the optical communication waveband (1650 nm) with an external bias. The dramatically enhanced photoresponse characteristics are attributed to narrowing of the band gap and a significantly decreased resistance, which originate from the enhancement of atomic orbital overlap owing to pressure-induced Pb-I bond contraction. These findings open up a new avenue toward designing self-driven and broadband photoelectric devices.

Crystal structure and Hirshfeld surface analysis of 4-(3-meth-oxy-phen-yl)-2,6-di-phenyl-pyridine.

The title compound, C24H19NO, was obtained via the reaction of (1E,2E)-3-(3-meth-oxy-phen-yl)-1-phenyl-prop-2-en-1-one with ethyl 2-oxo-propano-ate, using NH4I as a catalyst. The compound crystallizes in the monoclinic space group I2/a. In the mol-ecule, the four rings are not in the same plane, the pyridine ring being inclined to the benzene rings by 17.26 (6), 56.16 (3) and 24.50 (6)°. In the crystal, mol-ecules are linked by C-H⋯π inter-actions into a three-dimensional network. To further analyse the inter-molecular inter-actions, a Hirshfeld surface analysis was performed. Hirshfeld surface analysis indicates that the most abundant contributions to the crystal packing are from H⋯H (50.4%), C⋯H/H⋯C (37.9%) and O⋯H/H⋯O (5.1%) inter-actions.

Prognostic value of m6A regulators and the nomogram construction in glioma patients.

Although N6-methyladenosine (m6A) has been implicated in various biological functions in human cancers, its role in predicting the prognosis of glioma remains unclear. In this study, the transcriptome expression profiles and the clinical data of 961 patients were derived from the Chinese Glioma Genome Atlas (CGGA). We comprehensively evaluated the association between the expression of m6A regulators and the prognosis of glioma and established a 3-gene (YTHDF2, FTO, and ALKBH5) risk signature using least absolute shrinkage and selection operator (LASSO) analysis. Patients with a high-risk signature had significantly adverse prognoses. Gene set enrichment analysis (GSEA) analysis revealed that the G2M checkpoint, MTORC1 signaling, epithelial mesenchymal transition, and PI3K-AKT-mTOR signaling were significantly enriched in the high-risk group. Univariate and multivariate Cox regression analyses confirmed the independent prognostic value of this risk signature. We then constructed a nomogram for individualized prediction of overall survival (OS) by integrating clinicopathological features (age, World Health Organization [WHO] grade), treatment information (radiotherapy, temozolomide therapy), and m6A risk signature. The calibration curves showed excellent agreement between the predicted and actual probabilities for the 1-, 3-, and 5-year OS, with a C-index of 0.780 in the training cohort and 0.717 in the validation cohort. Altogether, our study elucidated the important role of m6A regulators in glioma prognosis, which is valuable for the selection of therapeutic methods and clinical management of patients with glioma.

Blink reflex: A practical test to evaluate the trigeminal nerve injury following percutaneous balloon compression for the treatment of trigeminal neuralgia.

OBJECTIVE: To evaluate the blink reflex (BR) in estimating the potential injury of trigeminal nerve following percutaneous balloon compression (PBC) surgery, and to determine the association between BR alterations and early surgical outcomes. METHODS: In this single-center, prospective before-and-after study, a total of 74 patients who had primary trigeminal neuralgia and scheduled for PBC between October 2020 and June 2021 were prospectively included. BR testing and facial sensory assessment were performed pre- and post-PBC. The latency and the area under the curve (AUC) of pre- and postoperative R1 (R1pre /R1post ) and R2 (R2pre /R2post ) were measured. RESULTS: The BR components were noticeably delayed or diminished following PBC. R1post was elicited in only 26 patients, and absent in 48 patients. The residual R1post had markedly reduced AUC (median difference [Hodges-Lehmann]: -59.5, 95% confidence interval [CI]: -217.5 to -6.9, p = 0.023). Compared with R2pre , the latency of R2post was considerably delayed (mean difference: 4.3, 95% CI: 2.9 to 5.7, p < 0.001) and the AUC was greatly suppressed (median difference [Hodges-Lehmann]: -388.4, 95% CI: -548.4 to -259.5, p < 0.001). After PBC, 58 patients had immediate total pain relief, and 16 had partial relief. The absence of R1post was found in 46 of 58 (79.3%) patients with complete remission, whereas in only 2 of 16 (12.5%) patients with partial relief. Association analysis showed that the absence of R1post was strongly associated with total pain relief (46/58 [79.3%] vs. 2/16 [12.5%], odds ratio [OR]: 26.8, 95% CI: 5.4 to 134.5, Cramér's V: 0.6, p < 0.001). The latency of R2post in patients with total relief was significantly delayed (mean difference: 2.5, 95% CI: 0.3 to 4.6, p = 0.028). Patients experienced graded facial numbness after PBC, of whom 31 reported mild numbness (Grades I-II) and 43 reported more severe numbness (Grades III-IV). The absence of R1post was significantly associated with facial numbness severity, 33/43 (76.7%) in Grades III-IV vs. 15/31 (48.4%) in Grades I-II (OR: 0.284, 95% CI: 0.105 to 0.771, Cramér's V: 0.3, p = 0.012). In patients with more severe numbness, the latency of R2post was significantly delayed (mean difference: 2.7, 95% CI: 0.1 to 5.3, p = 0.043), and the reduction of AUC was much greater (median difference [Hodges-Lehmann]: 17.2, 95% CI: 0.5 to 35.4, p = 0.041). CONCLUSION: Both R1 and R2 were significantly diminished after PBC and these alterations were associated with early surgical outcomes, suggesting that the BR is useful in evaluating trigeminal injury following PBC and could provide objective information about early prognosis.

A noisy chaotic neural network for solving combinatorial optimization problems: stochastic chaotic simulated annealing.

Recently Chen and Aihara have demonstrated both experimentally and mathematically that their chaotic simulated annealing (CSA) has better search ability for solving combinatorial optimization problems compared to both the Hopfield-Tank approach and stochastic simulated annealing (SSA). However, CSA may not find a globally optimal solution no matter how slowly annealing is carried out, because the chaotic dynamics are completely deterministic. In contrast, SSA tends to settle down to a global optimum if the temperature is reduced sufficiently slowly. Here we combine the best features of both SSA and CSA, thereby proposing a new approach for solving optimization problems, i.e., stochastic chaotic simulated annealing, by using a noisy chaotic neural network. We show the effectiveness of this new approach with two difficult combinatorial optimization problems, i.e., a traveling salesman problem and a channel assignment problem for cellular mobile communications.