近日,郑州大学化学学院卢思宇副教授课题组在碳点可控制备及其复合材料研究领域取得新进展。建立了一种以碳点为构筑单元制备碳化聚合物点与纳米晶杂化材料的普适方法。相关结果以“A General Route to Prepare Low-Ruthenium-Content Bimetallic Electrocatalysts for pH-Universal Hydrogen Evolution Reaction by Using Carbon Quantum Dots”为题发表在化学类顶尖期刊《Angewandte Chemie International Edition》上,第一作者为郑州大学博士研究生刘源,通讯作者为卢思宇副教授和中科院理化所张铁锐教授,郑州大学为第一通讯单位。
氢是一种清洁的可再生能源,电催化水分解是生产氢气的最理想的技术之一。碳点由于小尺寸限域效应、优异的导电性能和边缘效应,成为理想的催化剂载体。本文成功实现了碳点负载钌(Ru)基双金属电催化剂的可控制备,其中Ru的含量仅为5.93μg Ru cm-2。催化剂在1 M KOH、0.5 M H2SO4和1 M PBS中,达到10 mA cm-2所需的过电位分别仅为13、58和18 mV,是已报道的无铂电催化剂中最佳的催化活性之一。该研究也是课题组在碳点研究领域上的又一突破。
该研究得到了国家自然科学基金、中国博士后基金、郑州大学青年专项基金的支持。
全文链接: https://doi.org/10.1002/anie.201913910
Abstract
A challenging but pressing task to design and synthesize novel, efficient, and robust pH‐universal hydrogen evolution reaction (HER) electrocatalysts for scalable and sustainable hydrogen production through electrochemical water splitting. Herein, we report a facile method to prepare an efficient and robust Ru‐M (M=Ni, Mn, Cu) bimetal nanoparticle and carbon quantum dot hybrid (RuM/CQDs) for pH‐universal HER. The RuNi/CQDs catalysts exhibit outstanding HER performance at all pH levels. The unexpected low overpotentials of 13, 58, and 18 mV shown by RuNi/CQDs allow a current density of 10 mA cm−2 in 1 m KOH, 0.5 m H2SO4, and 1 m PBS, respectively, for Ru loading at 5.93 μgRu cm−2. This performance is among the best catalytic activities reported for any platinum‐free electrocatalyst. Theoretical studies reveal that Ni doping results in a moderate weakening of the hydrogen bonding energy of nearby surface Ru atoms, which plays a critical role in improving the HER activity.
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