原位构建P-N结复合材料及其可见光光催化性能

提高光催化过程中电子和空穴的提取和分离速率是提高光催化剂催化性能的关键技术之一。用浓硫酸剥离体相氮化碳得到石墨相g-C₃N₄,采用原位生长法制备花状g-C₃N₄/BiOBr P-N结复合材料,研究pH值对复合材料形貌的影响。利用XRD,SEM,EDS,TEM,UV-vis, BET等测试技术对所得样品的形貌、结构进行表征,讨论样品的光催化性能。结果表明:在g-C₃N₄/BiOBr复合材料内g-C₃N₄的[002]晶面和BiOBr的[001]晶面之间形成了异质结,可加速光生电子(e^-)和空穴(h⁺)的提取和分离。BiOBr和g-C₃N₄/BiOBr的禁带宽度分别为2.75,2.71 eV,复合材料的带隙减小,对可见光的吸收范围增强。BiOBr和g-C₃N₄/BiOBr复合材料的比表面积分别为1.27,6.43 m²/g,比表面积增大,增加催化反应活性位点。复合材料g-C₃N₄/BiOBr的光催化性能比纯g-C₃N₄和BiOBr更好,且重复使用效果佳。pH=8时制备的g-C₃N₄/BiOBr复合材料光催化效果最好,此时,对橙黄G、罗丹明B、甲基橙的光催化降解效率分别为91.00%,95.51%,96.72%。     

WS2/g-C3N4异质结光催化分解水制氢性能及机制

通过溶剂蒸发和二次高温煅烧石墨相碳化氮(g-C₃N₄)纳米片和WS₂纳米片混合物构建WS₂/g-C₃N₄异质结,该异质结保留g-C₃N₄和WS₂主体结构的同时,在界面处形成化学键,确保该异质结的化学稳定性和热稳定性。光催化分解水制氢实验表明,WS₂纳米片含量为3wt%时光催化制氢速率高达68.62 μmol/h,分别是g-C₃N₄纳米片和WS₂纳米片的2.53倍和15.29倍,表明异质结的构建可大幅提升g-C₃N₄的光催化性能,循环实验表明该异质结在5次循环实验后光催化性能没有明显下降,表明该异质结的稳定性较好。光电性能测试表明异质结的构建不仅提高激发电子的转移效率,同时抑制激发电子空穴的复合率,大幅提升激发电子的利用效率,致使光催化分解水制氢速率较g-C₃N₄纳米片和WS₂纳米片大幅提升。      

MOFs/g-C3N4复合光催化剂的研究进展

金属-有机框架材料(MOFs)和石墨相氮化碳(g-C₃N₄)在产氢、CO₂还原、Cr还原以及有机污染物降解方面表现出优异的光催化性能。将MOFs和g-C₃N₄结合构建二元或三元异质结,可以克服两种材料各自的缺点,进一步提高其材料在可见光或太阳光照射下的光催化性能。重点介绍了几种典型MOFs/g-C₃N₄复合材料的制备方法及其光催化性能,并展望了该研究领域发展前景和面临的挑战。     

硅藻土/g-C3N4/氧化石墨烯复合材料的制备及其光催化性能研究

采用半封闭一步热解方法，以三聚氰胺为前驱物制备g-C₃N₄,然后以圆筒状硅藻土(DE)为载体，合成DE/g-C₃N₄复合材料。并选取天然鳞片石墨为基本原料，运用Hummers法合成了氧化石墨烯(GO),在一定量的DE/g-C₃N₄粉末中加入不同质量分数的GO,得到DE/g-C₃N₄/GO三元复合光催化材料。通过SEM、BET、EDS、XRD、FT-IR对样品的晶体结构、形貌等进行表征，研究复合材料对罗丹明B溶液的光催化降解性能。结果表明，当GO的烯掺量为5%时，DE/g-C₃N₄/GO在可见光下，120min时，对RhB的降解率为93.74%,分别比DE/g-C₃N₄和g-C₃N₄提高了15.05%和31.03%。     

g-C3N4/高岭土复合材料的制备及其光催化性能研究

以水洗高岭土为载体, 采用盐酸对g-C₃N₄进行质子化处理, 通过浸渍法制备了g-C₃N₄/高岭土复合光催化材料。采用X射线衍射(XRD)、场发射扫描电镜(FESEM)和紫外-可见吸收光谱(UV-Vis)等手段对复合材料的晶体结构、微观形貌和光学性能进行了表征, 并以罗丹明B为目标降解物, 研究了复合材料在可见光下的光催化性能。结果表明: 当高岭土和g-C₃N₄的质量配比为6︰3时, g-C₃N₄/高岭土具有较优的光催化性能, 其光催化速率是纯g-C₃N₄的8.62倍; 高岭土和g-C₃N₄通过静电吸引力紧密结合在一起, 该复合结构能够有效地降低光生电子和空穴的复合几率, 改善了纯g-C₃N₄光催化材料的吸附性能, 进而有效提高了其光催化性能。     

可磁分离Fe3O4/g-C3N4复合材料的制备及其性能

为了利用Fe₃O₄的磁响应性及石墨相C₃N₄（g-C₃N₄）优良的光催化活性,首先采用高温热聚合法,以尿素为前驱体制备g-C₃N₄,然后采用水热法合成了可磁分离Fe₃O₄/g-C₃N₄复合材料。利用TEM、XRD、TGA、BET和振动样品磁强计（VSM）等多种测试手段表征分析Fe₃O₄/g-C₃N₄复合材料的形貌、晶型结构、比表面积、成分、饱和磁化强度等。通过模拟太阳光下Fe₃O₄/g-C₃N₄复合材料光催化吸附降解亚甲基蓝（MB）的实验,评价了Fe₃O₄/g-C₃N₄复合材料的吸附性能及光催化性能。结果表明,可磁分离Fe₃O₄/g-C₃N₄复合材料具有较大的比表面积,约为71.89 m²/g;且具有较好的磁性,饱和磁化强度为18.79 emu/g,可实现复合材料的分离回收;光照240 min时,Fe₃O₄/g-C₃N₄复合材料对MB的去除率为56.54%。所制备的Fe₃O₄/g-C₃N₄复合材料具有优良的吸附性能、光催化活性和磁性,并可通过外加磁场进行分离与回收。     

碳纳米球复合g-C3N4提升光催化降解酸性橙Ⅱ性能

基于g-C₃N₄构建的异质结光催化材料在降解有毒有害污染物方面体现出优良的效果。本研究通过水热法制备了一系列不同碳纳米球(Carbon nanospheres,CS)添加量的x-CS/g-C₃N₄ (x=4wt%、5wt%和7wt%)复合光催化剂,以氙灯光源模拟可见光,探究了x-CS/g-C₃N₄对酸性橙Ⅱ的光催化降解性能。结果表明:5wt% CS/g-C₃N₄的光催化活性最高,光催化反应150 min,酸性橙Ⅱ的降解率达到95%。表征结果表明,g-C₃N₄与CS具有类似的π-π共轭结构,易发生π-π堆积相互作用而有利于电子跃迁。二者复合后能有效增强g-C₃N₄对可见光的吸收效率,降低其表面/界面处的电荷转移电阻,显著增强载流子的传输能力。x-CS/g-C₃N₄可作为一种有效的可见光催化剂应用于有机染料降解,具有应用前景。      

Z型BiVO4/GO/g-C3N4复合材料的制备及其可见光下催化性能

Z-型光催化剂可以有效增强电荷分离, 从而改善光催化剂的活性。采用浸渍-煅烧和水热法两步制备Z型BiVO₄/GO/g-C₃N₄光催化剂, 并用不同手段对其进行表征。在BiVO₄/GO/g-C₃N₄的光催化过程中, GO纳米片作为BiVO₄和g-C₃N₄之间的快速传输通道, 可以抑制电子-空穴复合, 显著促进电荷分离, 提高三元异质结的氧化还原能力。与单组分或二元复合物相比, 该催化剂具有良好的光降解罗丹明B(RhB)的能力。在可见光照射下, 它能够在120 min内降解85% RhB, 空穴(h⁺)在反应中起主要作用。该工作为三元光催化剂体系提供了简单的制备方法, 其中g-C₃N₄通过GO与BiVO₄偶联, 光催化活性显著提高。     

g-C3N4/Cu-TiO2纳米球的制备及在紫外辅助芬顿中的催化性能表征

以一步法制备的7%(质量分数)Cu-TiO₂为基,利用水热法制备了不同质量分数的光催化性能优良的g-C₃N₄/Cu-TiO₂纳米球三元复合材料。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(UVVis DRS)等分析测试手段对样品的结构、形貌和光学性能进行表征。通过罗丹明B为模拟污染物,表征其在紫外光条件下的光催化性能,结果表明,所合成的催化剂为80～90 nm的光滑纳米球体,均匀分布在层片状的g-C₃N₄上,其中60%(质量分数)g-C₃N₄/Cu-TiO₂在紫外芬顿体系(0.1 mL 30%H₂O₂)内,在20 min内25 mg·L^-1罗丹明B降解率达到92.71%,在30 min达到100%。同时在pH范围2～8内具有同样高效的催化效果,显著提高了催化效率和适用pH范围。     

WO3/g-C3N4复合光催化剂制备及其可见光催化性能

将自制层状石墨相氮化碳(g-C₃N₄)和WO₃纳米片均匀混合,经煅烧制备WO₃/g-C₃N₄复合半导体。利用XRD、SEM、TEM、UV-Vis DRS和PL对其进行表征。结果表明,g-C₃N₄呈现类石墨烯状片层结构,WO₃为纳米片状结构,且分散在g-C₃N₄表面;与WO₃复合后,UV-Vis吸收边发生了红移,拓宽了g-C₃N₄对可见光的响应。以罗丹明B(RhB)为模拟污染物,考察WO₃/g-C₃N₄的光催化降解性能。WO₃/g-C₃N₄质量比为1∶5时,表现出最佳的光催化活性,可见光照60 min后,RhB降解率可达到94.9%。光催化剂具有良好的稳定性,重复使用6次后,RhB的降解率依然达到88.9%。光催化机制研究表明,超氧自由基(·O₂?)是光催化降解RhB的主要活性物种。      

g-C3N4/g-C3N4 isotype heterojunction as an efficient platform for direct photodegradation of antibiotic

A visible-light-driven g-C₃N₄/g-C₃N₄ isotype heterojunction photocatalyst was synthesized by one-step thermal treatment using urea and thiourea as the precursor. The photocatalytic activity of as-prepared photocatalyst was evaluated through the degradation of rhodamine B (RhB) and tetracycline hydrochloride (TC) under the visible light irradiation. The hybrid showed enhanced photocatalytic activity in photodegradating the applied pollutants as compared with single g-C₃N₄. When the ratio of urea to thiourea was 2:1, the prepared isotype heterojunction exhibited the highest photocatalytic activity and the photodegradation rates for RhB and TC were 99.8% and 95.1% after being visible light irradiated for 1 h and 4 h respectively. The enhanced photocatalytic performance of the isotype heterojunction is ascribed to the enhanced charge separation efficiency. After being reused for 5 times, the hybrid still showed excellent recyclability and chemical stability. Furthermore, NaI, BQ and IPA were used as the sacrificial agents for studying the surface reactions in the photocatalytic process. The method used in this work provides a new pathway to achieve more efficient degradation of antibiotics and to stimulate further studies in this important field.     

Co3O4负载rGO/g-C3N4臭氧光催化降解2,4-二氯苯氧乙酸活性研究

通过简单的水热法制备了Co₃O₄/rGO/g-C₃N₄催化剂,并在可见光照射下用于光催化臭氧氧化降解2,4-二氯苯氧乙酸(2,4-D)。利用XRD, SEM, TEM, XPS, UV-vis DRS, FT-IR和瞬态光电流对样品进行测试表征。研究表明,Co₃O₄, rGO和g-C₃N₄形成异质结后光生电子-空穴(e^--h⁺)对的分离效率,e^-的迁移能力以及光催化臭氧氧化活性都明显提升。此外,0.5Co₃O₄/0.25rGO/GCN对2,4-D具有100%的去除率,并具有最高反应速率(k=0.070 9 min^-1)。经过计算得出光催化臭氧氧化2,4-D的协同因子为3.91,表明光催化和臭氧氧化间具有较好的协同效应。活性组分的捕获实验结果表明h⁺和·OH是光催...     

二元碱金属共掺杂石墨相氮化碳的制备及光催化性能评价

以三聚氰胺为母体、以双组分碱金属为熔盐制备了钾-钠共掺杂石墨型氮化碳(g-C₃N₄)光催化剂,并用X射线衍射光谱(XRD)、紫外可见光谱(UV-Vis)、N₂吸附脱附、X光电子能谱(XPS)、荧光光谱(PL)等分析手段对产物进行了表征。结果表明,通过改变碱金属熔盐量,能将氮化碳价带(VB)能级从+1.55 V调控到+2.27 V、导带(CB)能级从-1.10 V调控到-0.27 V,同时碱金属的引入抑制了氮化碳晶粒的生长,降低了光生电子-空穴对的复合概率,提高了氮化碳的比表面积以及对可见光的吸收。以罗丹明B(RhB)为目标物研究了系列氮化碳在可见光驱动下的催化能力,实验结果表明,二元碱金属的掺入大大提高了催化剂降解和矿化罗丹明B的能力,并表现出良好的稳定性。     

Novel g-C<Subscript>3</Subscript>N<Subscript>4</Subscript> wrapped γ-Al<Subscript>2</Subscript>O<Subscript>3</Subscript> microspheres heterojunction for efficient photocatalytic application under visible light irradiation

The novel g-C₃N₄ wrapped γ-Al₂O₃ microspheres heterojunction was successfully prepared by a simple hydrothermal process followed by calcination. The photocatalytic performances of the composite were evaluated by the degradation of methyl orange (MO) and rhodamine B (RhB) under visible light irradiation. The obtained Al₂O₃/g-C₃N₄ heterojunction exhibited much higher photocatalytic activity compared to pure g-C₃N₄. The enhanced performance may be mainly attributed to the tight contact between the components of the heterostructure as well as the efficient transfer of photoinduced electrons from the valence band (VB) of g-C₃N₄ to the defect sites of γ-Al₂O₃. The trapping experiment results indicated that the ·O₂ ^? radicals and holes (h⁺) are main active species in the decomposition of MO. This work will provide new ideas for manipulation of high-performance heterojunction for practical photocatalysis applications in water pollution controls.     

碳纳米管修饰LaFeO3/TiO2复合材料的光催化性能与机理

采用超声辅助溶胶凝胶法制备了LaFeO₃颗粒,进一步以碳纳米管(CNTs)为基底和钛酸丁酯为前体,通过一步水热法煅烧合成CNTs/TiO₂/LaFeO₃(CTF)三元异质结光催化复合材料。通过扫描电子显微镜(SEM)、X射线衍射分析(XRD)、氮气吸附-解吸等温线(BET)、紫外-可见分光光度计(UV-Vis)、光致发光光谱(PL)等表征手段对材料的形貌与特征结构、比表面积和孔径结构以及光学特征进行了分析,并在紫外光下通过降解活性黑五(RB5)测试样品的光催化性能。结果表明,以CNTs作为载体,能够有效提升LaFeO₃/TiO₂复合材料的光催化性能。当CNTs在复合材料中的质量占比为5%时,150 W汞灯照射下RB5的50 min去除率可达99.5%。CNTs一方面通过增加复合材料的比较面积为催化反应的进行提供了更多的活性位点,更为重要的是,CNTs作为光生载流子传输的通道加快了电荷分离效率,提升了复合材料的降解能力和催化反应动力学进程。     

Preparation of a novel composite g-C3N4/TiO2/NiWO4 with enhanced photocatalytic activity toward the degradation of rhodamine B

A novel ternary heterojunction composite photocatalyst g-C₃N₄/TiO₂/NiWO₄ was fabricated using a simple hydrothermal method. The synthesized samples were characterized using X-ray diffraction (XRD), scanning electronic microscopy (SEM), energy-dispersive spectrum (EDS), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), ultraviolet–visible (UV–Vis) absorption spectra, photoluminescence (PL) spectra, transient photocurrent responses, and electrochemical impedance spectroscopies (EIS). The results indicated that the composite of g-C₃N₄/TiO₂/NiWO₄ had been successfully synthesized. By constructing a ternary heterojunction, the electron migration rate and light absorption of the material are further improved; the photogenerated electron–hole recombination is inhibited. The ternary composite photocatalyst shows the highest photocatalytic activity for the degradation of rhodamine B (RhB) than that of g-C₃N₄, TiO₂, NiWO₄, and g-C₃N₄/TiO₂ photocatalyst. The degradation efficiency of RhB using g-C₃N₄/TiO₂/NiWO₄ can reach 99% after visible-light irradiation for 40 min. Finally, the migration mechanism of charge carriers in the ternary system has been schematically illustrated by the active species capture experiment. Our research can pave the way for the fabrication of ternary heterojunction composite photocatalyst with high photocatalytic activity for the environmental contaminants treatment.

     

Facile synthesis of strontium molybdate coupled g-C3N4 composite for effective tetracycline and dyes degradation under visible light

This work was designed to synthesize SrMoO₄/g-C₃N₄ heterojunction for efficient degradation of tetracycline (TC) hydrochloride via photocatalysis. SrMoO₄/g-C₃N₄ samples were prepared through a grinding and roasting process. The prepared nanocomposite exhibited excellent visible-light-driven photocatalytic activity. The reaction rate of TC photodegradation reaches 0.0171 min^?1, which is 5.9 times higher than that of neat g-C₃N₄. The origin of the high photoactivity of SrMoO₄/g-C₃N₄ was investigated using a variety of characterization techniques including XRD, FT-IR, TG, SEM, TEM, XPS, DRS, Mott-Schottky, PL, PC, and EIS. Result showed that the added SrMoO₄ was closely loaded on the g-C₃N₄ surface, which is conducive to the electron transfer between SrMoO₄ and g-C₃N₄. Mott-Schottky analysis indicated that SrMoO₄ has a lower conduction band (CB) position than g-C₃N₄. As a result, photogenerated electrons in g-C₃N₄ can move to the CB of SrMoO₄ to hinder the recombination of charge carriers, thereby increasing the photocatalytic activity under visible light. The cycling test further suggested that the SrMoO₄/g-C₃N₄ heterojunction has good stability in the photocatalytic degradation of TC. Super oxygen radicals and holes are the main reactive species.     

Synthesis,Characterization and Photocatalytic Activity of TiO_2 Film/Bi_2O_3 Microgrid Heterojunction

TiO2 film modified by Bi2O3 microgrid array was successfully fabricated by using a microsphere lithography method.The structure and morphology of TiO2 film,Bi2O3 film and TiO2 film/Bi2O3 microgrid heterojunction were characterized through X-ray diffraction,atomic force microscopy and scanning electron microscopy.The optical transmittance spectra and the photocatalytic degradation capacity of these samples to rhodamine B were determined via ultraviolet-visible spectroscopy.The results indicated that the coupled system showed higher photocatalytic activity than pure TiO2 and Bi2O3 films under xenon lamp irradiation.The enhancement of the photocatalytic activity was ascribed to the special structure,which could improve the separation of photo-generated electrons and holes,enlarge the surface area and extend the response range of TiO2 film from ultraviolet to visible region.     

Enhancement of photocatalysis performance of CdIn2S4/g-C3N4 heterojunction by H2O2 synergism

A highly efficient binary CdIn₂S₄/g-C₃N₄ heterojunction photocatalyst was synthesized by a simple wet impregnation method. Photocatalytic system based on the synergistic action of binary CdIn₂S₄/g-C₃N₄ heterojunction and H₂O₂ was proposed to improve the degradation effect of dyes. The photocatalytic activity was evaluated by the degradation of methyl orange(MO) under visible light irradiation. The results demonstrated that contrasted to pure g-C₃N₄, the synthesized heterojunction can significantly improve the photocatalytic activity. After 120 min of irradiation by visible light, the photocatalytic efficiency of MO degradation of 7CIS/CN was 3.13 times higher than that of g-C₃N₄. When 60 mM H₂O₂ was added on this basis, the photocatalytic efficiency increased from 93.81 to 99.40%. The improvement of photocatalytic activity is attributed to the formation of binary CdIn₂S₄/g-C₃N₄ heterojunction to promote the transfer of photogenerated electron-hole pairs, and an appropriate amount of H₂O₂ as an electron trap further reduced the recombination rate of photogenerated electron-hole pairs. Active species capture experiments showed that ·O₂^? are the main active substances. Subsequently, the mechanism of photocatalytic degradation was proposed. This work provided a new efficient strategy for the degradation of industrial dye wastewater.

     

Super-Photothermal Effect-Mediated Fast Reaction Kinetic in S-Scheme Organic/Inorganic Heterojunction Hollow Spheres Toward Optimized Photocatalytic Performance

Using full solar spectrum for energy conversion and environmental remediation is a major challenge, and solar-driven photothermal chemistry is a promising route to achieve this goal. Herein, this work reports a photothermal nano-constrained reactor based on hollow structured g-C₃N₄@ZnIn₂S₄ core–shell S-scheme heterojunction, where the synergistic effect of super-photothermal effect and S-scheme heterostructure significantly improve the photocatalytic performance of g-C₃N₄. The formation mechanism of g-C₃N₄@ZnIn₂S₄ is predicted in advance by theoretical calculations and advanced techniques, and the super-photothermal effect of g-C₃N₄@ZnIn₂S₄ and its contribution to the near-field chemical reaction is confirmed by numerical simulations and infrared thermography. Consequently, the photocatalytic degradation rate of g-C₃N₄@ZnIn₂S₄ for tetracycline hydrochloride is 99.3%, and the photocatalytic hydrogen production is up to 4075.65 µmol h⁻¹ g⁻¹, which are 6.94 and 30.87 times those of pure g-C₃N₄, respectively. The combination of S-scheme heterojunction and thermal synergism provides a promising insight for the design of an efficient photocatalytic reaction platform.