片状石墨相氮化碳的制备及光催化性能研究

以三聚氰胺为前驱体,采用高温煅烧法、水热法预处理法、氨基修饰法以及氮气二次煅烧(热剥离法)制备g-C₃N₄,并对样品进行了结构表征与分析,并进行了光催化性能及稳定性测试。结果表明：四种制备方法对样品的光催化活性有显著的影响,热剥离法制备的样品有较好的光催化性能,氨基改性法制备的样品具有较好的稳定性能,可以多次重复使用。     

硫酸根对聚合氮化碳光催化活性的影响

在pH=1条件下分别加入硫酸根、硝酸根、磷酸根对三聚氰胺进行处理,采用高温煅烧法制备了一系列聚合氮化碳材料,并通过X射线衍射（XRD）、扫描电子显微镜（SEM）、紫外-可见漫反射光谱（UV-Vis DRS）等分析手段对样品进行了表征。以罗丹明B（RhB）为污染物,探究了在可见光下聚合氮化碳对RhB的光催化降解性能、稳定性以及降解机理。加入0.12 mol硫酸根处理的聚合氮化碳（CN-0.04SO₄^2-）在45 min内对RhB的降解率为99.1%,其伪一级动力学常数是未加硫酸根的23.0倍,硫酸根能有效地增强聚合氮化碳的光催化活性。CN-0.04SO₄^2-经过3次循环实验对RhB的降解率略有下降,说明其具有良好的稳定性。活性物种捕获实验表明,影响光催化降解RhB的主要活性物种是·O₂^-和·OH。     

聚合氮化碳的制备、改性及光催化还原二氧化碳性能研究

由过量二氧化碳（CO₂）排放导致的温室效应使得全球气候变暖问题日益紧迫,在“双碳”背景下,如何资源化利用CO₂尤为重要。光催化还原CO₂生成化学品和燃料是有望同时解决能源危机和环境问题的途径。非金属半导体聚合氮化碳（PCN）具有可见光响应、化学稳定性高、易于制备等优点,在光催化领域备受关注,但由传统热聚合方法得到的PCN存在比表面积小、电子-空穴对复合严重、对可见光吸收范围窄等不足之处。介绍了光还原CO₂的反应机理和PCN的结构,总结了PCN的制备方法以及提升其光还原CO₂性能的手段,包括形貌调控、异原子掺杂、缺陷工程和构建异质结等。最后,对目前PCN材料在CO₂光还原反应研究中存在的问题进行了分析,并对未来发展方向进行了展望。     

甲酸铵处理对氮化碳光催化性能的影响

石墨相氮化碳(g-C₃N₄)作为环境友好型材料在半导体光催化领域广受关注,然而未经改性的g-C₃N₄光吸收范围窄,仅能对太阳光谱中蓝紫光区响应,同时比表面积小,且光生载流子分离及迁移速率慢,导致光催化性能不佳。本文以g-C₃N₄为研究对象,将甲酸铵(NH₄HCO₂)和硫脲(CH₄N₂S)按不同比例混合,在马弗炉中520℃下高温煅烧(升温4 h保温2 h),制得C元素掺杂的石墨相氮化碳。g-C₃N₄中掺杂C元素可提高光吸收能力、调整电荷密度、促进光生载流子解离,从而显著提高其光催化效率。通过降解模拟污染物罗丹明B(RhB)发现,当n(CH₄N₂S)∶n(NH₄HCO₂)=1∶0.04时表现出最好的光催化活性,其对罗丹明B的降解效率几乎能达到1...     

氮化碳分散液的制备及其光催化性能

以尿素热解得到的块状体相氮化碳为前驱体,采用硫酸质子化结合超声剥离的方法制备氮化碳纳米片分散液,考察不同工艺条件如溶剂种类、稳定剂浓度、氮化碳原料浓度、超声时间等对其分散性的影响。通过UV-Vis、FTIR、XRD、SEM、BET等方法对分散液的浓度、结构、微观形貌和比表面积进行表征分析;并以亚甲基蓝为目标降解物,研究其在可见光照射下的光催化性能。结果表明,以水为溶剂、ρ(稳定剂)=1.2 mg/mL、ρ(氮化碳)=1.0 mg/mL、超声时间为18 h制备的氮化碳纳米片分散液性能最好,其在可见光照射180 min后对亚甲基蓝的光催化降解率达77.93%。     

氮化碳接枝L-谷氨酰胺分子实现高效光催化产氢和降解性能

将尿素和L-谷氨酰胺(Lg)作为前体材料,使用冷冻-煅烧法成功将Lg分子链接枝到了氮化碳(CN)的边缘,制备了具有优异光催化性能Lg接枝修饰的多孔氮化碳(LCN)光催化剂。通过X射线衍射光谱(XRD)、扫描电子显微镜(SEM)、傅里叶变换红外光谱(FTIR)、X射线光电子能谱(XPS)等表征测试方法对样品的形貌结构以及光催化性能进行了测试。结果表明,Lg分子链的引入不仅能够增加材料的比表面积,提供更多的活性位点,同时还可以有效促进光生电子的快速分离和转移,从而获得优异的光催化活性。在可见光的照射下,最优质量比的LCN-10光催化剂在析氢测试过程中产氢速率高达658μmol/(g·h),约是纯相CN的3倍。并且在光降解盐酸四环素(TCH)和左氧氟沙星(LEV)的测试中,LCN-10也表现出良好的催化活性,在60min内对TCH和LEV的光降解率达到了98%及85%。这项工作为CN基光催化材料的表面修饰与性能优化提供了新的视角。     

质子化氮化碳的制备及其复合材料的光催化性能

分别采用硫酸、盐酸和硝酸对尿素热解得到的体相块状石墨相氮化碳(g-C_3N_4)进行质子化改性,超声剥离得到氮化碳纳米片,考察3种质子化氮化碳纳米片对亚甲基蓝染料的光催化降解性能,利用XRD、FT-IR、SEM、BET、UV-DRS、UV-VIS等对其结构、形貌、比表面积、禁带宽度进行分析。结果表明,硫酸改性后的g-C_3N_4比表面积最大(60. 9 m~2·g~(-1)),亚甲基蓝降解效果最好,降解率为46. 7%,相比于体相块状g-C_3N_4的29. 2%提高了17. 5个百分点。以硫酸质子化改性的g-C_3N_4为前驱体,采用搅拌法制备得到质子化g-C_3N_4/石墨烯复合材料,其光催化降解亚甲基蓝的降解率为81. 7%,较硫酸质子化g-C_3N_4提高了35. 0个百分点。     

氧掺杂氮化碳的制备及对农田环境残留农药的降解性能

[目的]构建适用于多菌灵等4种烟-稻轮作农田常用农药的可见光催化降解技术,并阐释降解机制,为缓解农田环境农药残留造成的采收期作物农残超标问题提供理论和技术支撑。[方法]通过高温聚合法制备氧掺杂氮化碳纳米材料,通过扫描电子显微镜等表征技术分析材料微观结构。通过光催化降解试验,评价并筛选出降解性能最优的材料,同时研究复杂因素对降解过程的影响。[结果]氧元素掺杂可有效提高氮化碳纳米材料对目标农药的光催化降解性能,最优材料OCN_0.1对多菌灵可见光下1 h内降解率即可达到94.6%,通过活性物种捕获试验,证实在目标农药的降解过程中,活性物种的贡献度排序为h⁺>¹O₂>·O₂^-。OCN_0.1不仅能有效降解水环境残留农药,在作物生长阶段,喷施OCN_0.1材料48 h后,农残降解率最大也可提高39.95%。[结论]制备获得的OCN_0.1纳米材料,可有效降低农田环境及作物中的农药残留水平,具有良...     

硫酸胍制备多孔石墨型氮化碳及其光催化降解苯酚

为了增加比表面积和提高催化活性,一种无毒和易得的前驱体硫酸胍被首次用于制备石墨型氮化碳(g-C_3N_4)。用X射线粉末衍射、红外光谱、扫描电镜、透射电镜、N_2吸附-脱附、光电子能谱、紫外-可见光吸收光谱和荧光光谱对所得多孔g-C_3N_4进行表征。与由三聚氰胺为前驱体制备的体相g-C_3N_4相比,硫酸胍为前驱体制备的多孔g-C_3N_4具有更高的比表面积、发达的孔结构和较好的光电性能。以光催化降解苯酚为模型反应考察催化剂性能,结果表明,所得多孔g-C_3N_4的催化活性明显高于体相g-C_3N_4。优异的光催化性能和简单的合成方法使硫酸胍制备的多孔g-C_3N_4可广泛用于环境和能源领域。     

Kapok fiber modified carbon nitride photocatalytic degradation of organic pollutants

A kapok fiber (KF) modified graphite phase carbon nitride (g-C₃N₄) catalyst was prepared by a one-step pyrolysis method, and the photocatalytic degradation of organic pollutants was investigated. The structure and optical properties of KF-CN were characterized by XRD, UV-Vis DRS, TEM, PL, XPS, FT-IR and N₂ adsorption-desorption. The nitrogen adsorption-desorption isotherm results show that the presence of the mesoporous structure can improve the specific surface area of KF-CN. Elemental analysis characterization indicates the biochar modification is conductive to increase the C/N ratio of KF-CN. The XPS characterization also indicates that the introduction of carbon element can change the chemical environment of N element in the lattice of g-C₃N₄ and thus increases the electron density of N element. The photocatalytic degradation of phenol experiment was carried out to investigate the performance of as-prepared kapok fiber modified graphite carbon nitride photocatalysts by using high-pressure sodium lamp as visible light source. The results show the KF(5%)-CN(600) displayed the highest phenol degradation rate constant of 0.259 h^-1, which is 4.2 times of that of neat g-C₃N₄.The activity of KF(5%)-CN(600) does not decrease significantly after 5 cycles, hinting its excellent catalytic stability and structural stability. The possible reaction mechanism was proposed.     

木棉纤维改性氮化碳光催化降解有机污染物

采用一步热解法制备了木棉纤维(KF)改性的石墨相氮化碳(g-C₃N₄)催化剂,并考察了催化剂光催化降解有机污染物的性能。采用XRD、UV-Vis DRS、FT-IR、TEM、XPS、N₂吸附-脱附、PL表征对催化剂进行了结构、形貌、光学性能测试。结果表明,KF改性可以提高催化剂的比表面积,更大的比表面积可以提供更多的活性位点来参与光催化降解过程。UV-Vis DRS结果表明KF改性可以缩小催化剂的禁带宽度,提高催化剂对光能的吸收。在可见光下,KF改性的g-C₃N₄基催化剂对苯酚降解速率常数为0.259 h^-1,是纯g-C₃N₄的4.2倍,且具有优异的催化稳定性和结构稳定性。     

漂浮型氮化碳光催化剂CNx@mEP的制备及性能

针对氮化碳粉末光催化剂在应用过程中存在难以回收、光催化效率不高的问题,本研究采用“浸渍-煅烧”方法,以膨胀珍珠岩为载体,制备了一种方便回收、可多次利用的漂浮型氮化碳光催化剂CNx@mEP。采用扫描电镜（SEM）、X射线衍射仪（XRD）、X射线光电子能谱仪（XPS）、全自动比表面及孔径分析仪（BET）、傅里叶红外光谱仪（FTIR）以及紫外可见近红外漫反射测试（UV-vis）对CNx@mEP进行了分析。分别通过染料降解实验和有害藻类去除实验考察了催化剂的光催化性能。当双氰胺使用量与膨胀珍珠岩载体的质量比为2∶1时得到的CN2@mEP材料光催化性能最好,当催化剂使用量为4g/L时,在可见光下4h降解67.2%的罗丹明B、86.8%的刚果红、31.2%的甲基橙染料和35%的铜绿微囊藻。漂浮型氮化碳光催化剂经过3次重复利用后,仍保持较为稳定的去除效率。     

Tuning and thermal exfoliation graphene-like carbon nitride nanosheets for superior photocatalytic activity

In this work, ultrathin graphene-like carbon nitride nanosheets with rich nanoporous and excellent hydrophilic characteristics were synthesized by a simple and effective thermal exfoliation of bulk g-C₃N₄. In order to fully understand the effect of thermal exfoliation conditions on the texture, surface state, and photocatalytic activity of the resulting g-C₃N₄, a series of exfoliated g-C₃N₄ were prepared by adjusting the thermal exfoliation temperature and time. The detailed characterization and analysis distinctly suggested that increasing exfoliation temperature led to a large number of nitrogen vacancies and increased specific surface area, further prolonging exfoliation time, the thermal exfoliation degree was enhanced, more carbon vacancies and enlarged pore volume formed in the resulting products. Further, the exfoliation degree and photocatalytic ability of the resultant products were enhanced by increasing thermal exfoliation temperature and time. The optimized ultrathin graphene-like carbon nitride nanosheets exhibited a 89.6% degradation efficiency for Rh6G only in 10 min, which was much faster than other such nanosheets reported in previous literature.     

Tailoring the bandgap of N-rich graphitic carbon nitride for enhanced photocatalytic activity

Nitrogen - rich graphitic carbon nitride (Ng-C₃N₄) with improved photocatalytic activity was engineered using a facile post-annealing treatment of pristine g-C₃N₄ in N₂ atmosphere. The thermal annealing did not modify the crystal structure, vibrational modes, or morphology of the N-rich g-C₃N₄ (Ng-C₃N₄). However, it decreased the crystallinity by broadening the dominant X-ray diffraction (XRD) peak and increased the surface area and mesoporous nature because of the formation of carbon vacancies. Diffuse reflectance spectroscopy indicated that the bandgap of the annealed Ng-C₃N₄ decreased from 2.82 to 2.77 eV compared to pristine g-C₃N₄. The increase of nitrogen content in the annealed Ng-C₃N₄ was quantified by X-ray photoelectron spectroscopy (XPS), which was also used to examine the formation of carbon vacancies. Photocurrent and electrochemical impedance spectroscopy measurements showed that the annealed Ng-C₃N₄ had higher light absorption capacity than the pristine g-C₃N₄. The photocatalytic performance of the samples was investigated for the degradation of crystal violet (CV) under ultra-violet light irradiation. The annealed Ng-C₃N₄ sample exhibited superior photodegradation of CV over pristine g-C₃N₄.     

Pomelo biochar as an electron acceptor to modify graphitic carbon nitride for boosting visible-light-driven photocatalytic degradation of tetracycline

In this study, biochar (BC) derived from pomelo was prepared via a high-temperature calcination method to modify the graphitic carbon nitride (g-C₃N₄) to synthesize the BC/g-C₃N₄ composite for the degradation of the tetracycline (TC) antibiotic under visible light irradiation. The experimental results exhibit that the optimal feeding weight ratio of biochar/urea is 0.03:1 in BC/g-C₃N₄ composite could show the best photocatalytic activity with the degradation rate of tetracycline is 83% in 100?min irradiation. The improvement of photocatalytic activity is mainly attributed to the following two points: (i) the strong bonding with π-π stacking between BC and g-C₃N₄ make the photogenerated electrons of light-excited g-C₃N₄ transfer to BC, quickly and improve the separation efficiency of carriers; (ii) the introduction of BC reduces the distance for photogenerated electrons to migrate to the surface and increases the specific surface area for providing more active sites. This study provides a sustainable, economical and promising method for the synthesis of photocatalytic materials their application to wastewater treatment.     

硫酸根改性g-C3N4制备与催化性能研究

采用酸水热后处理法制备了具有优异光催化合成双氧水性能的硫酸根改性石墨相氮化碳纳米棒催化剂。采用XRD、N2吸附脱附、UV-Vis、FTIR、SEM、XPS、TPD、EIS及PL对催化剂进行表征。结果显示：硫酸根的引入改变了催化剂的结构性质，光学性质和氧气吸附能力。所制备的硫酸根改性氮化碳催化剂的双氧水平衡浓度为2.7 mmol/L，是纯氮化碳的2.7倍。