本文選題：生物炭 + 重金屬　； 參考：《蘭州交通大學(xué)》2017年博士論文

【摘要】：隨著城市化和工業(yè)化的快速發(fā)展,土壤重金屬污染的不斷加劇已經(jīng)成為不容忽視的環(huán)境問題。生物炭(Biochar)是生物質(zhì)在限氧條件下熱解制備的富碳顆粒。生物炭由于其具有豐富的表面官能團(tuán)和發(fā)達(dá)的孔隙結(jié)構(gòu)等特征使其對重金屬具有較強(qiáng)的吸附固定化性能,生物炭作為固定化材料修復(fù)重金屬污染土壤已成為環(huán)境和土壤領(lǐng)域的研究熱點(diǎn)之一。論文簡要介紹了土壤重金屬污染及其修復(fù)技術(shù)研究進(jìn)展,重點(diǎn)評(píng)述了生物炭吸附重金屬的特性及機(jī)制和生物炭在重金屬污染土壤固定化修復(fù)中的應(yīng)用研究進(jìn)展。針對生物炭施加到黃土后對重金屬的吸附固定性能與生物炭結(jié)構(gòu)之間的構(gòu)效關(guān)系尚不明確,生物炭施加對黃土中重金屬鎘(Cd)的植物有效性與植物吸收Cd含量的相關(guān)關(guān)系不清等問題,本文選擇玉米秸稈生物質(zhì)為代表制備生物炭,通過SEM-EDS、FTIR、XRD、XPS、比表面積測定和元素分析等手段表征了生物炭的表面性質(zhì)和結(jié)構(gòu)特征;研究了生物炭對Cd的吸附特性和機(jī)制,探討了生物炭對共存重金屬的競爭吸附機(jī)制;進(jìn)一步采用表面改性方法制備了氨基修飾玉米秸稈生物炭,探明了氨基修飾生物炭對Cd的吸附機(jī)制;在此基礎(chǔ)上,揭示了生物炭施入黃土后對Cd的吸附固定性能與生物炭結(jié)構(gòu)之間的構(gòu)效關(guān)系;最后探究了生物炭施入Cd污染黃土后對Cd賦存形態(tài)分布和Cd植物有效性的影響機(jī)制。研究結(jié)果為區(qū)域土壤重金屬污染控制提供科學(xué)依據(jù)。論文的主要結(jié)果及創(chuàng)新性如下:(1)揭示了玉米秸稈生物炭與Cd的相互作用機(jī)制,發(fā)現(xiàn)生物炭表面的含氧官能團(tuán)對Cd的絡(luò)合作用是其吸附Cd的主要機(jī)制。生物炭吸附Cd前后的XRD圖譜未發(fā)現(xiàn)新的衍射峰,表明生物炭吸附Cd后沒有沉淀物質(zhì)產(chǎn)生,即表面沉淀作用不是生物炭吸附Cd的主要機(jī)制。同時(shí),生物炭吸附Cd前后的FTIR譜圖上的羥基(—OH)和羰基(C=O)特征峰波數(shù)發(fā)生偏移、峰強(qiáng)降低,表明—OH和C=O對Cd產(chǎn)生了表面絡(luò)合作用。研究生物炭吸附Cd前后的XPS特征,結(jié)果發(fā)現(xiàn),生物炭吸附Cd的過程中其表面含氧官能團(tuán)對應(yīng)的結(jié)合能分別向高能量偏移0.2 eV,表明生物炭表面含氧官能團(tuán)與Cd形成Cd—R鍵(R表示為—COO、—CO等)。此外,溶液平衡pH值在生物炭吸附Cd后由5.4降低至5.1,進(jìn)一步證實(shí)了生物炭表面官能團(tuán)與Cd形成配合物。Cd、Cu和Zn在生物炭上的競爭吸附行為表明,生物炭對Cd、Cu和Zn的吸附性能與重金屬自身的物理化學(xué)性質(zhì)有關(guān)。氨基修飾生物炭對Cd的吸附機(jī)制主要為生物炭表面的氨基官能團(tuán)和含氧官能團(tuán)與Cd的絡(luò)合作用,且生物炭氨基官能團(tuán)對Cd的結(jié)合能力強(qiáng)于含氧官能團(tuán)對Cd的結(jié)合能力。(2)率先研究了生物炭對黃土中Cd吸附固定作用的構(gòu)效關(guān)系。發(fā)現(xiàn)生物炭自身的理化性質(zhì)對施加生物炭黃土吸附Cd有顯著影響,生物炭的極性是影響施加生物炭黃土吸附Cd最關(guān)鍵的因素。添加不同比例生物炭的黃土對Cd的吸附結(jié)果表明,添加生物炭黃土對Cd的吸附性能高于黃土對Cd的吸附性能,且隨著生物炭添加比例的增大,生物炭添加黃土對Cd的吸附性能顯著增強(qiáng)。添加不同原料制備生物炭的黃土對Cd的吸附性能也存在較大差異,向黃土中添加秸稈生物炭對Cd的吸附性能優(yōu)于糞質(zhì)生物炭和玉米芯生物炭。同時(shí)研究發(fā)現(xiàn),不同溫度制備的生物炭的理化性質(zhì)有較大差異,而生物炭的極性指標(biāo)(O+N)/C和添加生物炭黃土吸附Cd的模型參數(shù)KF呈現(xiàn)良好的正相關(guān)關(guān)系,而生物炭比表面積與添加生物炭黃土吸附Cd的性能之間沒有顯著的相關(guān)關(guān)系。(3)研究了玉米秸稈生物炭施入Cd污染黃土后對黃土中Cd的賦存形態(tài)的影響以及黃土中Cd賦存形態(tài)和玉米體內(nèi)Cd含量的關(guān)系。發(fā)現(xiàn)向Cd污染黃土施加生物炭可顯著降低黃土中有效態(tài)Cd的含量,其作用機(jī)制包括生物炭的石灰效應(yīng)改變黃土中Cd的賦存形態(tài)、生物炭吸附固定作用降低Cd的有效濃度。生物炭對Cd污染黃土性質(zhì)及Cd賦存形態(tài)分布的影響研究結(jié)果表明,生物炭施加可顯著升高土壤pH值、土壤陽離子交換量(CEC)和土壤有機(jī)質(zhì)(SOM)含量,同時(shí)可提高黃土中脲酶和堿性磷酸酶的活性。向Cd污染黃土施加生物炭促使Cd由不穩(wěn)定的有效態(tài)轉(zhuǎn)化為穩(wěn)定的殘?jiān)鼞B(tài)。同時(shí),玉米根部與地上部Cd含量與黃土中有效態(tài)Cd含量呈極顯著正相關(guān)(P0.01),與殘?jiān)鼞B(tài)Cd含量呈極顯著負(fù)相關(guān)(P0.01),生物炭施入Cd污染黃土顯著降低了玉米根部和地上部的Cd含量(P0.05)。
[Abstract]:With the rapid development of urbanization and industrialization, the increasing pollution of heavy metals in soil has become an environmental problem that can not be ignored. Biological carbon (Biochar) is a carbon rich particle prepared by the pyrolysis of biomass under the condition of oxygen limiting. Biological carbon has the characteristics of heavy metal with its rich surface functional groups and the pore structure of hair. It has become one of the hot topics in the field of environment and soil to repair heavy metal contaminated soil as a immobilized material. The paper briefly introduces the research progress of soil heavy metal pollution and its remediation technology. It focuses on the characteristics and mechanism of bio carbon adsorbed heavy metals and the heavy metals in biological carbon. The research progress in the application of immobilized remediation of contaminated soil. The relationship between the adsorption fixed performance of heavy metals and the structure of biological carbon after the application of the biological carbon to the loess is not clear. The relationship between the plant availability of heavy metal cadmium (Cd) in the Loess and the absorption of Cd in the plant is not clear. Maize straw biomass was used as the representative to prepare biological carbon. The surface properties and structural characteristics of biological carbon were characterized by means of SEM-EDS, FTIR, XRD, XPS, specific surface area measurement and element analysis. The adsorption characteristics and mechanism of biological carbon to Cd were studied, and the competitive adsorption mechanism of biological carbon to coexisting heavy metals was discussed, and surface modification was further used. Methods the amino modified maize straw bio carbon was prepared, and the adsorption mechanism of amino modified biological carbon to Cd was explored. On this basis, the relationship between the adsorption fixed properties of Cd and the structure of biological carbon was revealed after the biological charcoal was applied into the loess. Finally, the distribution of Cd and the Cd plants were explored after the biological charcoal was applied to the Cd polluted loess. The main results and innovations of this paper are as follows: (1) the interaction mechanism of maize straw bio carbon and Cd was revealed, and the cooperative use of oxygen containing functional groups to Cd on the surface of biochar was the main mechanism for its adsorption of Cd. Before Cd was adsorbed by biological carbon No new diffraction peak was found in the XRD map, indicating that no precipitate was produced after adsorption of Cd by biological carbon. That is, the surface precipitation is not the main mechanism for the adsorption of Cd by biological charcoal. At the same time, the number of hydroxyl (- OH) and carbonyl (C=O) peaks on the FTIR spectrum before and after the adsorption of Cd is offset and the peak intensity decreases, indicating that OH and C=O have produced Cd. The surface complexing effect. Study the XPS characteristics before and after adsorption of Cd by biological carbon. It is found that the corresponding binding energy of oxygen functional groups on the surface of biological carbon migration to high energy is 0.2 eV respectively, indicating that oxygen functional groups on the surface of carbon dioxide and Cd form Cd R bonds (R represents COO, CO, etc.). Besides, the pH value of the solution balance is absorbed in biological carbon. The adsorption of Cd,.Cd, Cu and Zn on biological carbon showed that the adsorption properties of Biocharcoal on Cd, Cu and Zn were related to the physical and chemical properties of heavy metals. The adsorption mechanism of amino modified carbon to Cd was mainly the ammonia on the surface of Cd. The combination of basic functional group and oxygen containing functional group with Cd, and the binding ability of biological carbon amino functional groups to Cd is stronger than that of oxygen containing functional groups on Cd. (2) the structure effect relationship of the adsorption and fixation of Cd in loess was first studied. It was found that the physical and chemical properties of biological charcoal have significant influence on the application of Cd to the adsorption of Cd on the biological carbon loess. The polarity of biological charcoal is the most important factor affecting the adsorption of Cd on the adsorption of Biocharcoal loess. The adsorption of Cd by adding different proportions of biological carbon to the Loess shows that the adsorption performance of Cd is higher than that of the loess to Cd, and with the increase of the proportion of biological charcoal, the adsorption property of biological charcoal to Cd is remarkable. The adsorption performance of Cd by adding different raw materials for biological carbon was also greatly different. The adsorption performance of Cd by adding straw bio carbon to Huang Tuzhong was better than that of fecal carbon and corn cob. Meanwhile, the physical and chemical properties of biological charcoal prepared at different temperatures were different, and the polarity index of biological carbon (O+N) was also found. /C and the model parameter KF of adding biological carbon loess to Cd showed good positive correlation, but there was no significant correlation between the specific surface area of biological carbon and the performance of adding bio carbon loess to the adsorption of Cd. (3) the effects of maize straw bio carbon into the Cd contaminated loess and the occurrence of Cd in the Loess and the occurrence of Cd in loess were studied. The relationship between morphology and the content of Cd in maize was found. It was found that applying biological carbon to Cd contaminated loess could significantly reduce the content of effective Cd in loess. The mechanism of its action included the lime effect of biological charcoal to change the form of Cd in loess, and the adsorption and fixation of Biocharcoal to reduce the effective concentration of Cd. The properties of Cd contaminated loess and the existence of Cd form by biological carbon. The results of the influence of the state distribution showed that the soil pH value increased significantly, the soil cation exchange (CEC) and the soil organic matter (SOM) content, and the activity of urease and alkaline phosphatase in the loess. The application of bio carbon to the Cd polluted loess promoted the transformation of Cd from the unstable effective state to the stable residue state. There was a significant positive correlation between the Cd content of rice root and the upper part of the ground and the content of effective Cd in the loess (P0.01), which had a significant negative correlation with the residue Cd content (P0.01). The content of Cd in the root and upper part of the maize (P0.05) was significantly reduced by the application of the biological carbon into the Cd polluted loess.
【學(xué)位授予單位】：蘭州交通大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2017
【分類號(hào)】：X53

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