The structure of metal-water interface at the potential of zero charge from density functional theory-based molecular dynamics

J. Le thanks the College of Physical Sciences, University of Aberdeen for a PhD studentship. Calculations were performed on ARCHER, the UK’s high end computing resource, as part of a grant to the UKCP consortium, and on the computing cluster Maxwell at the University of Aberdeen. J. C. is grateful for funding support by the National Natural Science Foundation of China (Grants No. 21373166 and 21621091), and the Thousand Youth Talents Program of China.Peer reviewedPostprin

Theoretical insight into vibrational spectra of metal-water interfaces from density functional theory based molecular dynamics

Acknowledgements J. C. is grateful for funding support from the National Natural Science Foundation of China (Grants No. 21373166 and 21621091), and the Thousand Youth Talents Program of China.Peer reviewedPostprin

Determining Potentials of Zero Charge of Metal Electrodes versus the Standard Hydrogen Electrode from Density-Functional-Theory-Based Molecular Dynamics

J. Le thanks University of Aberdeen for a PhD studentship. We thank the UKCP consortium program on ARCHER, and Maxwell at University of Aberdeen for computing time. J. C. is grateful for funding support by the National Natural Science Foundation of China (Grant No. 21373166 and 21621091), and the Thousand Youth Talents Program of China.Peer reviewedPublisher PD

GTWS-MLrec: global terrestrial water storage reconstruction by machine learning from 1940 to present

Terrestrial water storage (TWS) includes all forms of water stored on and below the land surface, and is a key determinant of global water and energy budgets. However, TWS data from measurements by the Gravity Recovery and Climate Experiment (GRACE) satellite mission are only available from 2002, limiting global and regional understanding of the long-term trends and variabilities in the terrestrial water cycle under climate change. This study presents long-term (i.e., 1940–2022) and relatively high-resolution (i.e., 0.25∘) monthly time series of TWS anomalies over the global land surface. The reconstruction is achieved by using a set of machine learning models with a large number of predictors, including climatic and hydrological variables, land use/land cover data, and vegetation indicators (e.g., leaf area index). The outcome, machine-learning-reconstructed TWS estimates (i.e., GTWS-MLrec), fits well with the GRACE/GRACE-FO measurements, showing high correlation coefficients and low biases in the GRACE era. We also evaluate GTWS-MLrec with other independent products such as the land–ocean mass budget, atmospheric and terrestrial water budget in 341 large river basins, and streamflow measurements at 10 168 gauges. The results show that our proposed GTWS-MLrec performs overall as well as, or is more reliable than, previous TWS datasets. Moreover, our reconstructions successfully reproduce the consequences of climate variability such as strong El Niño events. The GTWS-MLrec dataset consists of three reconstructions based on (a) mascons of the Jet Propulsion Laboratory of the California Institute of Technology, the Center for Space Research at the University of Texas at Austin, and the Goddard Space Flight Center of NASA; (b) three detrended and de-seasonalized reconstructions; and (c) six global average TWS series over land areas, both with and without Greenland and Antarctica. Along with its extensive attributes, GTWS_MLrec can support a wide range of geoscience applications such as better understanding the global water budget, constraining and evaluating hydrological models, climate-carbon coupling, and water resources management. GTWS-MLrec is available on Zenodo through https://doi.org/10.5281/zenodo.10040927 (Yin, 2023)

Electric-field-induced selective catalysis of single-molecule reaction

随着单分子电学检测技术的迅速发展，分子电子学的研究不再局限于分子电子学器件的构筑及其电学性质的测量，而且扩展到单分子尺度化学反应过程的探索。然而目前相关的研究仍然局限于理论计算方面，在单分子尺度上实时监测和调控化学反应的活性和选择性是化学领域的长期目标和挑战。针对这一挑战，洪文晶教授课题组与程俊教授课题组合作，自主研发了精密科学仪器，将单个有机分子定向连接在两个末端尺寸为原子级的电极之间，解决了化学反应中分子取向控制的问题.理论计算结果证实了定向电场可以有效地稳定化学反应的过渡态，从而降低反应能垒。该研究工作在化学化工学院洪文晶教授、程俊教授、能源材料化学协同创新中心（iChEM）刘俊扬副研究员的共同指导下完成，由硕士研究生黄晓艳、iChEM博士研究生唐淳、博士研究生李洁琼以及兰州大学的陈力川博士作为共同第一作者，化学化工学院师佳副教授、陈招斌高级工程师、夏海平教授和田中群教授，萨本栋微纳研究院杨扬副教授、环境与生态学院白敏冬教授以及兰州大学张浩力教授参与了研究工作的讨论并给予指导，博士后乐家波、博士研究生郑珏婷、张佩（已毕业）、李瑞豪、李晓慧也参与了研究工作。Oriented external electric fields (OEEFs) offer a unique chance to tune catalytic selectivity by orienting the alignment of the electric field along the axis of the activated bond for a specific chemical reaction; however, they remain a key experimental challenge. Here, we experimentally and theoretically investigated the OEEF-induced selective catalysis in a two-step cascade reaction of the Diels-Alder addition followed by an aromatization process. Characterized by the mechanically controllable break junction (MCBJ) technique in the nanogap and confirmed by nuclear magnetic resonance (NMR) in bottles, OEEFs are found to selectively catalyze the aromatization reaction by one order of magnitude owing to the alignment of the electric field on the reaction axis. Meanwhile, the Diels-Alder reaction remained unchanged since its reaction axis is orthogonal to the electric fields. This orientation-selective catalytic effect of OEEFs reveals that chemical reactions can be selectively manipulated through the elegant alignment between the electric fields and the reaction axis.This work was supported by the National Key R&D Program of China (2017YFA0204902), the National Natural Science Foundation of China (21722305, 21703188, 21673195, 21621091, 51733004, 51525303, and 91745103), the China Postdoctoral Science Foundation (2017M622060), and the Young Thousand Talents Project of China. 该工作得到国家自然科学基金委（21722305、21703188、21673195、51733004、51525303、91745103），国家重点研发计划课题（2017YFA0204902），中国博士后面上基金（2017M622060）的资助，以及固体表面物理化学国家重点实验室、醇醚酯化工清洁生产国家工程实验室、能源材料化学协同创新中心的支持