三嗪类除草剂阿特拉津被长期广泛用于去除阔叶和禾本科杂草，因其半衰期长、具有生物累积性等特点对人类健康和环境生态安全构成严重威胁。如何高效去除环境中残留的阿特拉津受到国内外研究学者的广泛关注。近年来，生物炭因其独特的表面特性、氧化还原特性等广泛用于环境污染治理领域。研究表明，生物质原料的类型对生物炭的性能影响很大。非木质类污泥生物质具有高水分、高灰分、低热值、低堆积密度和较多的孔隙等特点，而木质纤维素类农业秸秆生物质的特点则为低水分、低灰分、高热值、高堆积密度和较少的孔隙。因此，单一生物质原料自身特性对热解过程的制约及其解决方案的探索也备受关注。本研究通过共热解污泥和大豆秸秆的混合物，探究制备条件对生物炭吸附能力与催化降解阿特拉津效能的影响并揭示泥杆共热解生物炭活化过硫酸盐降解阿特拉津的反应机制，主要结果与结论如下：

（1）探究不同泥秆比例（0∶1、1∶0、1∶1、1∶2、1∶5、1∶10）、不同热解温度（450 ℃、600 ℃、700 ℃、800 ℃、900 ℃）下所制备系列生物炭对阿特拉津吸附性能的影响，结果表明泥秆共热解生物炭对阿特拉津的吸附效果总体上优于单大豆秸秆生物炭（W0S1 900）以及单污泥生物炭（W1S0 900）。其中900 ℃，污泥和大豆秸秆比为1:2时所制备的泥秆共热解生物炭（W1S2 900）对阿特拉津的吸附效果最好，最终吸附率可达51.01%。SEM-EDS结果显示W0S1 900为自然纤维管束结构，W1S0 900表面存在大量的团聚纳米颗粒，而W1S2 900表面保存了天然的多孔结构，且负载少量纳米颗粒。W1S2 900主要由C、N、O、Cu、Zn五种元素组成，其中C元素占比为46.90%，N元素占比为19.86%，O元素占比为20.65%，Cu元素占比为5.56%，Zn元素占比为7.03%。BET分析可得W1S2 900相较W0S1 900、W1S0 900比表面积更大，为547.251 m²/g。

（2）以大豆秸秆生物炭、污泥生物炭为对照，深入探究代表性共热解生物炭对阿特拉津的吸附性能。W0S1 900、W1S0 900、W1S2 900对阿特拉津的吸附均分为两个阶段，前5 h为快速吸附过程，并在12 h内达到吸附平衡状态。通过比较动力学模型相关系数R²发现，二级动力学模型更适合描述三种生物炭对阿特拉津的吸附行为。而在吸附等温线研究中，Freundlich吸附等温线模型更适合解释三种生物炭对阿特拉津的吸附过程，并因此推断该吸附过程可能以多层吸附的形式发生在非均匀表面上，而不是简单的发生在光滑均匀表面上的单层吸附。W1S2 900在Freundlich模型中的1/n值均小于1，说明W1S2 900对阿特拉津的吸附过程容易发生。由吸附热力学结果可知，W1S2 900较W0S1 900、W1S0 900反应自发进行的程度较高。且三种生物炭体系均为吸热反应，随着温度的升高，反应体系中分子运动的无序性升高。以上这些研究结果均表明，通过污泥与大豆秸秆共热解可以实现生物炭对阿特拉津的高效吸附。

（3）进一步探究泥秆共热解生物炭活化过硫酸盐降解阿特拉津的效能发现，W1S2 900活化过硫酸盐对阿特拉津的降解率为94.90%，降解速率常数为0.04282，这可能是因为污泥的掺杂带入大量金属元素，使其对PS的活化更强，产生的自由基更多。通过探究不同反应条件对降解效果的影响可得，在W1S2 900-PS体系中，W1S2 900投加量为50 mg，PS剂量为1.5 mM，室温中性条件下其对阿特拉津的降解效果最好。又探究了共存阴离子（Cl^-、CO₃^2-、HCO₃^-）、腐殖酸（HA）对W1S2 900-PS体系阿特拉津降解效果的影响，结果表明Cl^-和HA基本不会对降解效果产生影响，而CO₃^2-、HCO₃^-以1 mM以上的高浓度存在时才会对降解效果产生较大影响。在连续循环试验中比较了W1S2 900、W0S1 900、W1S0 900的可重复利用性，5次试验后W1S2 900对阿特拉津的去除率仍能保持在50%左右，而W1S0 900、W0S1 900最终只剩10%左右的去除率，表明W1S2 900相较W0S1 900、W1S0 900稳定性更好。

（4）通过对于反应前后生物炭表面变化、反应后溶液中阿特拉津降解产物和体系中活性物质的分析，深入揭示泥杆共热解生物炭活化过硫酸盐降解阿特拉津的反应机制。FTIR检测得到W1S2 900在波长约1602 cm⁻¹处产生了C=O的伸缩振动峰，在波长约1413 cm^-1处出现了-CN的伸缩振动峰，在波长约1112 cm⁻¹处产生了C-O的伸缩振动峰，这些官能团的存在表明其可能发生了苯环取代使其极性减弱，从而对阿特拉津的去除能力增强。XPS分析结果也表明其存在C=O、C-O，和吡啶氮、吡咯氮，而吡啶氮和吡咯氮被认为具有较高的催化活性。XRD分析出其高度石墨化结构。EPR检测到了W1S2 900-PS体系中的主要活性物质^·OH、SO₄^·−、¹O₂强峰，这几种活性物质都对阿特拉津的降解起关键作用。最后通过LC-MS检测了阿特拉津的主要代谢产物，发现阿特拉津的降解路径虽不完全相同，但都是进行脱氯或支链上的烷基，且途径可相互转化。

Atrazine, a triazine herbicide, has been widely used for removing broad-leaved and gramineous weeds for a long time. Due to its long half-life and bioaccumulation, it poses a serious threat to human health and environmental ecological security. How to efficiently remove residual atrazine in the environment has received widespread attention from domestic and foreign researchers. In recent years, biochar has been widely used in the field of environmental pollution control due to its unique surface characteristics, redox properties, and other properties. Research has shown that the type of biomass raw material has a significant impact on the performance of biochar. Non woody sludge biomass has the characteristics of high moisture content, high ash content, low calorific value, low bulk density, and more pores, while woody cellulose agricultural straw biomass has the characteristics of low moisture content, low ash content, high calorific value, high bulk density, and fewer pores. Therefore, the constraints of the characteristics of a single biomass raw material on the pyrolysis process and the exploration of solutions have also attracted much attention. This study investigated the effects of preparation conditions on the adsorption capacity of biochar and the catalytic degradation efficiency of atrazine by co-pyrolysis of sludge and soybean straw mixture, and revealed the reaction mechanism of activated persulfate degradation of atrazine by biochar co-pyrolysis of sludge and straw. The main results and conclusions are as follows:

(1) Exploring the effects of different sludge and straw ratios (0∶1, 1∶0, 1∶1, 1∶2, 1∶5, 1∶10) and pyrolysis temperatures (450 ℃, 600 ℃, 700 ℃, 800 ℃, 900 ℃) on the adsorption performance of atrazine in a series of biochars prepared, the results showed that the adsorption effect of sludge and straw co-pyrolysis biochar on atrazine was generally better than that of single soybean straw biochar (W0S1 900) and single sludge biochar (W1S0 900). The sludge and straw co-pyrolysis biochar (W1S2 900) prepared at a ratio of 1:2 between sludge and soybean straw at 900 ℃ showed the best adsorption effect on atrazine, with a final adsorption rate of 51.01%. The SEM-EDS results show that W0S1 900 has a natural fiber bundle structure, with a large number of aggregated nanoparticles on the surface of W1S0 900, while W1S2 900 retains its natural porous structure and is loaded with a small amount of nanoparticles. W1S2 900 is mainly composed of five elements: C, N, O, Cu, and Zn, with C accounting for 46.90%, N accounting for 19.86%, O accounting for 20.65%, Cu accounting for 5.56%, and Zn accounting for 7.03%. BET analysis shows that W1S2 900 has a larger specific surface area of 547.251 m²/g compared to W0S1 900 and W1S0 900.

(2) In depth exploration of the adsorption performance of representative co-pyrolysis biochar for atrazine, using soybean straw biochar and sludge biochar as controls. The adsorption of atrazine by W0S1 900, W1S0 900, and W1S2 900 is divided into two stages, with the first 5 hours being a rapid adsorption process and reaching adsorption equilibrium within 12 hours. By comparing the correlation coefficient R² of the kinetic models, it was found that the second-order kinetic model is more suitable for describing the adsorption behavior of the three biochars on atrazine. In the study of adsorption isotherms, the Freundlich adsorption isotherm model is more suitable for explaining the adsorption process of atrazine by three types of biochar, and therefore infers that the adsorption process may occur in the form of multi-layer adsorption on non-uniform surfaces, rather than simply single-layer adsorption on smooth and uniform surfaces. The 1/n values of W1S2 900 in the Freundlich model are all less than 1, indicating that the adsorption process of atrazine by W1S2 900 is prone to occur. According to the thermodynamic results of adsorption, W1S2 900 exhibits a higher degree of spontaneous reaction compared to W0S1 900 and W1S0 900. And all three biochar systems are endothermic reactions, and as the temperature increases, the disorder of molecular motion in the reaction system increases. The above research results all indicate that efficient adsorption of atrazine by biochar can be achieved through co- pyrolysis of sludge and soybean straw.

(3) Further exploration of the efficiency of activated persulfate degradation of atrazine by biochar co-pyrolysis of sludge and straw revealed that the degradation rate of atrazine by W1S2 900 activated persulfate was 94.90%, with a degradation rate constant of 0.04282. This may be due to the incorporation of a large amount of metal elements into the sludge, which enhances its activation of PS and generates more free radicals. By exploring the influence of different reaction conditions on the degradation effect, it can be concluded that in the W1S2 900-PS system, the W1S2 900 dosage is 50 mg, the PS dosage is 1.5 mM, and the degradation effect of atrazine is best under neutral conditions at room temperature. We also investigated the effects of coexisting anions (Cl^-, CO₃^2-, HCO₃^-) and humic acid (HA) on the degradation efficiency of atrazine in the W1S2 900-PS system. The results showed that Cl - and HA had little effect on the degradation efficiency, while CO₃^2- and HCO₃^- only had a significant impact on the degradation efficiency when they were present at high concentrations above 1 mM. The reusability of W1S2 900, W0S1 900, and W1S0 900 was compared in continuous cycle tests. After 5 experiments, W1S2 900 still maintained a removal rate of about 50% for atrazine, while W1S0 900 and W0S1 900 only had a final removal rate of about 10%, indicating that W1S2 900 has better stability compared to W0S1 900 and W1S0 900.

(4) By analyzing the surface changes of biochar before and after the reaction, the degradation products of atrazine in the solution after the reaction, and the active substances in the system, the reaction mechanism of activated persulfate degradation of atrazine by sludge and straw co-pyrolysis biochar is revealed in depth. FTIR detection showed that W1S2 900 exhibited a stretching vibration peak of C=O at a wavelength of approximately 1602 cm^-1, a stretching vibration peak of -CN at a wavelength of approximately 1413 cm^-1, and a stretching vibration peak of C-O at a wavelength of approximately 1112 cm^-1. The presence of these functional groups suggests that it may have undergone benzene ring substitution, leading to a decrease in polarity and an enhancement of its ability to remove atrazine. The XPS analysis results also indicate the presence of C=O, C-O, pyridine nitrogen and pyrrole nitrogen are considered to have high catalytic activity. XRD analysis revealed its highly graphitized structure. EPR detected strong peaks of the main active substances ^·OH, SO₄^·−, and ¹O₂ in the W1S2 900-PS system, all of which play a critical role in the degradation of atrazine. Finally, the main metabolites of atrazine were detected by LC-MS, and it was found that although the degradation pathways of atrazine were not completely the same, they all involved dechlorination or alkyl groups on the branched chain, and the pathways could be converted into each other.

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