Valorization of soybean plant wastes in preparation of N-doped biochar for catalytic ozonation of organic contaminants: Atrazine degradation performance and mechanistic considerations
Valorization of soybean plant wastes in preparation of N-doped biochar for catalytic ozonation of organic contaminants: Atrazine degradation performance and mechanistic considerations
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DOI：
10.1016/j.cej.2023.145153
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发表时间：
2023-08
影响因子：
15.1
通讯作者：
Shiwen Dong;X. Shen;Qingqing Guo;Haijun Cheng;S. Giannakis;Zhiqiao He;Lizhang Wang;Da Wang;Shuang Song;Jun Ma
中科院分区：
文献类型：
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作者：
Shiwen Dong;X. Shen;Qingqing Guo;Haijun Cheng;S. Giannakis;Zhiqiao He;Lizhang Wang;Da Wang;Shuang Song;Jun Ma
选择生物质来源是至关重要的，因为不同的植物或组织可能表现出不同的质地和化学性质。然而，很少有研究者对同一植物不同组织在炭化后的催化活性进行比较。大豆是世界范围内广泛种植的作物，经常遭受病虫害。收获的大豆储存不当会导致发霉和浪费。以大豆废组织为前驱体制备了大豆生物炭（SB）、大豆壳生物炭（SBS）和大豆秸秆生物炭（SS）催化剂，显著提高了臭氧氧化催化降解阿特拉津的效率。用SB的表面积（kobs/SBET）归一化的比反应速率常数表明，SBET不影响生物炭的催化氧化性能。表征结果表明，离域π-电子、含氮官能团和含氧官能团在催化臭氧化过程中起着关键作用，这些活性位点对自由基和非自由基活性氧（ROS）的生成，包括羟基自由基（•OH）、超氧自由基（O2•−）和单重态氧（1O2）的产生都有助于阿特拉津的降解。与SBS和SS相比，SB具有最高的吡啶N含量，最高的羰基（-C = O）含量，最强的离域电子密度和电子给体能力，这是其优越的催化性能的原因。这些生物炭上的活性位点增强了臭氧的吸附和分解，加速了电子转移过程，产生更多的活性氧，实现了高效的污染物消除。总的来说，在“废物处理废物”概念的指导下，本研究为农业废弃大豆植物的回收和再利用提供了有价值的替代方案，证明了衍生的生物炭可能被用作基于高级氧化过程的催化剂。
Selecting the biomass source is critical because different plants or tissues may exhibit varying textures and chemical properties. However, few researchers have compared the catalytic activity of different tissues from the same plant after carbonization. Soybean is widely cultivated worldwide and always suffers from pests and diseases. The inappropriate storage of harvested soybeans leads to mildew and its wastage. Herein, soybean biochar (SB), soybean shell biochar (SBS), and soy straw biochar (SS) catalysts were prepared using waste soybean plant tissues as precursors, which drastically improved the degradation efficiency of atrazine in catalytic ozonation. The specific reaction rate constant normalized by the surface area (kobs/SBET) of SB during catalytic ozonation indicated the catalytic performance of biochar was not affected just bySBET. The characterization results showed that the delocalized π-electrons, nitrogen-, and oxygen-containing functional groups played key roles in catalytic ozonation, and contributions of these active sites to the generation of both radical and nonradical reactive oxygen species (ROS) including hydroxyl radicals (•OH), superoxide radicals (O2•−), and singlet oxygen (1O2) contributed to atrazine degradation. Compared with SBS and SS, SB contained the highest pyridine N content, the highest carbonyl group (–C = O) content, the strongest delocalized electron density, and electron donor ability, which was responsible for its superior catalytic performance. Such active sites on biochar enhanced the ozone adsorption and decomposition, accelerated the electron transfer process to produce more ROS, and achieved efficient pollutant elimination. Overall, guided by the “waste treating waste” concept, this study provided a valuable alternative in the recycling and reuse of agricultural waste soybean plants, proving that the derived biochar could be potentially used as a catalyst for advanced oxidation processes-based applications.