Theoretical Studies of Metal-N-C for Oxygen Reduction and Hydrogen Evolution Reactions in Acid and Alkaline Solutions

单原子催化剂（SAC）由于其低成本和在各种电催化反应中潜在的高催化活性而被认为是铂族金属的有前景的替代材料,但仍然缺乏对不同金属氮碳材料催化剂之间活性差异的原子机理的理解。在此,通过实验和理论研究相结合,研究了非贵金属氮碳材料（Me-N-C,Me = Fe和Co）作为模型催化剂,以探索在普遍的pH值下氧还原反应（ORR）和氢析出反应（HER）的催化活性以及相对应的反应机理。原子理论模拟表明,Fe-N-C具有比Co-N-C高的ORR活性,这是因为其速率决定步骤的反应势垒较低,而HER的活性趋势却相反。我们的模拟结果与实验观察结果一致。Single atom catalysts (SAC) have been regarded as the promising alternatives to platinum group metals due to their low costs and potentially high catalytic activities in various electrocatalytic reactions. The atomic mechanism understanding of activity discrepancy among different metal and nitrogen co-doped carbon-based catalysts is still lacking. Here, non-precious metal and nitrogen co-doped carbons (Me-N-C, Me = Fe and Co) as the model catalysts are investigated by combining experimental and theoretical studies to explore the catalytic activities and corresponding reaction mechanisms toward oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) at universal pHs. Atomic theoretical simulations suggest that Fe-N-C has higher ORR activity than Co-N-C due to its lower reaction barrier of the rate-determining step, while the activity trend is reversed for HER. Our simulation results are consistent with experimental observations.通讯作者:秦雪苹,邵敏华E-mail:[email protected];[email protected]:Xue-PingQin,Min-HuaShaoE-mail:[email protected];[email protected].化工与生物工程系,香港科技大学,香港 9990772.能源材料与电信研究中心,魁北克 加拿大1. Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, China2. INRS-énergie, Matériaux et Télécommunications, 1650 Boulevard Lionel Boulet, Varennes, Québec, Canada J3X 1S

Effects of elevated temperature on soil respiration in a coastal wetland during the nongrowing season in the Yellow River Delta, China

冬季土壤呼吸能释放生长季所固存的碳,因而在陆地碳循环中占有重要地位。随着全球气候变暖,平均地表温度将升高0.3–4.8℃,且冬季增温更加明显,而温度的升高会促进更多CO2的释放。另外,滨海湿地地下水位浅,淡咸水交互作用明显,增温能引起土壤表层盐分升高,从而影响土壤呼吸。该研究以黄河三角洲滨海湿地为研究对象,采用红外辐射加热器模拟增温,研究了该地区非生长季土壤呼吸的日动态及季节动态,同时探讨了土壤呼吸对环境因子的响应机制。结果显示:日动态中,增温与对照的土壤呼吸速率变化趋势一致,为单峰曲线;在平均日变化中,整个非生长季不同处理的土壤呼吸速率无显著差异,而土壤温度和土壤盐分均为增温大于对照,并且土..

25MeV/u Kr辐照下PET薄膜的损伤机制研究；Damage Mechanism of PET Irradiated by 25 MeV/u Kr Ions

通过25MeV/u86Kr离子辐照叠层结晶聚对苯二甲酸乙二醇酯膜(PET),在不同的电子能损(3.407.25keV/nm)和离子注量(5×10113×1012ions/cm2)辐照条件下,对Kr离子在PET中引起的辐照损伤效应进行了研究。借助傅里叶变换红外光谱分析,通过对样品的红外吸收峰进行扣除基底后的Lorentz拟合,分析了与主要官能团对应的吸收峰强度的变化趋势,研究了化学结构与组分在重离子辐照下的变化规律;利用X射线衍射光谱仪测量,研究了Kr离子在PET潜径迹中引起的非晶化过程,并通过对吸光度和非晶化强度随离子注量的指数衰减规律的分析,获得了不同电子能损离子辐照PET时主要官能团的损伤截面和非晶化截面及对应的潜径迹半径