Aqueous-phase oxygen evolution reaction (OER) is the bottleneck of water splitting. The formation of the O−O bond involves the generation of paramagnetic oxygen molecules from the diamagnetic hydroxides. The spin configurations might play an important role in aqueous-phase molecular electrocatalysis. However, spintronic electrocatalysis is almost an uncultivated land for the exploration of the oxygen molecular catalysis process. Herein, we present a novel magnetic Fe III site spin-splitting strategy, wherein the electronic structure and spin states of the Fe III sites are effectively induced and optimized by the Jahn−Teller effect of Cu 2+ . The theoretical calculations and operando attenuated total reflectance-infrared Fourier transform infrared (ATR FT-IR) reveal the facilitation for the O−O bond formation, which accelerates the production of O 2 from OH − and improves the OER activity. The Cu 1 −Ni 6 Fe 2 −LDH catalyst exhibits a low overpotential of 210 mV at 10 mA cm −2 and a low Tafel slope (33.7 mV dec −1 ), better than those of the initial Cu 0 −Ni 6 Fe 2 −LDHs (278 mV, 101.6 mV dec −1 ). With the Cu 2+ regulation, we have realized the transformation of NiFe−LDHs from ferrimagnets to ferromagnets and showcase that the OER performance of Cu−NiFe−LDHs significantly increases compared with that of NiFe−LDHs under the effect of a magnetic field for the first time. The magnetic-fieldassisted Cu 1 −Ni 6 Fe 2 −LDHs provide an ultralow overpotential of 180 mV at 10 mA cm −2 , which is currently one of the best OER performances. The combination of the magnetic field and spin configuration provides new principles for the development of highperformance catalysts and understandings of the catalytic mechanism from the spintronic level.

Highly efficient and low-cost oxygen reduction reaction electrocatalysts play key roles in the development of advanced energy conversion and storage devices, such as fuel cells and metal–air batteries. Herein, a facile strategy of synthesizing cobalt single atoms anchored on an ultrathin N-doped carbon nanosheet electrocatalyst (marked as CoSAs/N-CNS) via an in situ g-C3N4 template strategy was reported. Impressively, benefiting from highly active Co–Nx sites and highly porous and ultrathin nanosheet morphology which has rich edges and more three-phase boundaries, the as-synthesized CoSAs/N-CNS exhibits markedly enhanced ORR activities under alkaline conditions with half-wave potential (E 1/2) as high as 0.91 V vs RHE, as well as durability of ∼67 h. Furthermore, compared with Pt/C, the CoSAs/N-CNS-based Zn–air battery presents outstanding discharge–charge performance, larger power density of 157.7 mW cm–2, and robust durability with a slight decay after 150 h (900 cycles). The experimental and theoretical results fully show the advantages of CoSAs/N-CNS, which also provides a new insight for the design and development of high-performance atomically dispersed metal active site electrocatalysts toward ORR.

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Objective: This study evaluated the survival outcomes of young (<50 years) and elderly patients (>80 years) with high-risk prostate cancer (PCa) postradical local treatments. Materials and Methods: We identified <50 and >80-year-old patients with high-risk PCa between 2004 and 2015 in the Surveillance, Epidemiology, and End Results database. The patients aged 65 and 66 years were also identified as the control group. The propensity-score matching method was adopted to compare the young and elderly patients with the control group. Kaplan–Meier analysis and Cox regression were conducted to evaluate the PCa-specific survival (PCSS) and overall survival. Results: A total of 17726 patients were identified, and 3355 were under 50 years old, whereas 4798 of them were >80 years old. The young patient group (<50 years) had similar PCSS with the control group (65–66 years) in both the overall cohort (hazard ratio [HR]: 0.88, 95% confidence interval [CI] [0.73–1.06], P = 0.132) and matched cohort (HR: 0.96, 95% CI [0.74–1.24], P = 0.527). Young patients with both high-risk and very high-risk PCa after radical prostatectomy (RP) treatment had apparent longer mean cancer-specific survival time than those after external-beam radiotherapy (EBRT) and/or brachytherapy (BT) treatment (high-risk group: 153.38 ± 0.82 months vs. 149.72 ± 3.03 months; very high-risk group: 148.3 ± 1.84 months vs. 139.33 ± 3.25 months). For the elderly patients (>80 years), the PCSS outcomes were significantly worse than the control group (65–66 years) in both overall cohort (HR: 2.69, 95% CI [2.31–3.13], P < 0.001) and matched cohort (HR: 1.61, 95% CI [1.34–1.94], P < 0.001). Patients receiving RP treatment had similar PCSS outcomes with those receiving EBRT and/or BT in the high-risk PCa group (139.45 ± 9.98 months vs. 139.41 ± 1.84 months), and better PCSS in very high-risk PCa group (132.73 ± 13.56 months vs. 128.82 ± 3.43 months). Conclusion: The PCSS outcomes of young PCa patients (<0 years) were identical to those of the control group (65–66 years). RP had similar or better PCSS benefits than EBRT and/or BT in both young (<50 years) and elderly patients (>80 years).

摘要超薄二维金属有机框架(Two-dimensional metal-organic frameworks (2D MOFs))具有较大的比表面积和 开放的催化活性中心, 在电催化反应中具有潜在的应用价值. 本工作报道了一种溶剂热法制备的具有开放位点的 超薄2D Ni-MOF纳米片阵列及其在电催化苯甲醇氧化(Electrocatalytic benzyl-alcohol oxidation (EBO))方面的应 用. 作为一种高性能的EBO电催化剂, 2D Ni-MOF表现出较低的过电位和优异的化学耐久性, 仅需要约1.50 V的 电位即可达到250 mA cm −2 , 苯甲醇氧化效率达85%. 2D Ni-MOF纳米片阵列相比于同样具有超薄结构的2D Ni (OH) 2 纳米片阵列, 反应过电势降低约35 mV(@50 mA cm −2 ), 具有更快的反应动力学. 在同一恒电位下进行苯甲 醇氧化反应时, 具有更高的响应电流, 并且在连续电解20000 s后, 可保留25 mA cm −2 的电流密度, 接近Ni(OH) 2 纳 米片的两倍, 表现出更优异的电催化活性. Ni-MOF纳米片中的Ni具有更高的氧化态, 在EBO反应中更容易转化成 活性位点NiOOH, 使得其在更低的电位下能有效催化苯甲醇的电氧化反应. 这一结果为进一步设计高性能电催化 苯甲醇氧化反应电催化剂提供新的视角.