State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China; Research Center of the Ministry of Education for High Gravity Engineering and Technology, Beijing University of Chemical Technology, Beijing 100029, China.
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China; Research Center of the Ministry of Education for High Gravity Engineering and Technology, Beijing University of Chemical Technology, Beijing 100029, China.
J Colloid Interface Sci. 2020 Jul 1;571:100-108. doi: 10.1016/j.jcis.2020.03.035. Epub 2020 Mar 10.
The cellulose, which is one of the most abundant solid by-products of agriculture and forestry industry, has been successfully tested for the synthesis of nitrogen and phosphorus co-doped carbon-based metal-free catalysts (NPC) via freeze-drying the mixture of cellulose crystallite and ammonium phosphate, followed by annealing of the hydrogel under nitrogen atmosphere at 800 °C for 2 h. Different techniques including TEM, SEM, FTIR and XPS spectroscopy have been applied to characterize the as-prepared NPC, which presents flake-like morphology with N and P doping levels of 4.3 atom% and 10.66 atom%, respectively. The NPC exhibits excellent catalytic activity for the reduction of p-nitrophenol (p-NP). The turnover frequency (TOF) of the reduction of p-NP is as high as 2 × 10 mmol·mg·min and the apparent kinetic rate constant was calculated as 0.0394 min at room temperature. The catalytic mechanism is proposed by combining the density functional theory calculation and analysis of the experimental results. These findings open up new possibilities of valorization for cellulose-based by-product and treatment of p-NP-based wastewater.
纤维素是农业和林业工业中最丰富的固体副产物之一,已成功通过冷冻干燥纤维素微晶和磷酸铵的混合物来合成氮磷共掺杂碳基无金属催化剂(NPC),然后在氮气气氛下将水凝胶在 800°C 下退火 2 小时。采用 TEM、SEM、FTIR 和 XPS 光谱等不同技术对所制备的 NPC 进行了表征,其呈现出具有 N 和 P 掺杂水平分别为 4.3 原子%和 10.66 原子%的片状形态。NPC 对 p-硝基苯酚(p-NP)的还原表现出优异的催化活性。p-NP 还原的转化率频率(TOF)高达 2×10 mmol·mg·min,在室温下计算的表观动力学速率常数为 0.0394 min。通过结合密度泛函理论计算和实验结果分析,提出了催化机制。这些发现为基于纤维素的副产物的增值和基于 p-NP 的废水处理开辟了新的可能性。