木质素基N,S-CQDs的制备及其在Fe^(3+)检测中的应用

以木质素磺酸钠为碳源和硫源,低共熔溶剂(DES)为氮源和反应溶剂制备了一种氮、硫双掺杂的碳量子点(N,S-CQDs)。制备的N,S-CQDs的粒径分布均匀,平均粒径为4.95 nm,量子产率达到了35.7%,量子产率大幅提升。制备的N,S-CQDs对Fe^(3+)具有优异的敏感性,可用于Fe^(3+)的定量检测,检测限为0.25μmol·L^(-1),检测范围是0~200μmol·L^(-1)。

N503萃取Fe^3＋工艺研究

用N503对Fe3+溶液进行萃取实验研究。结合试验详细阐述了萃取相Fe质量分数与水相中Fe3+质量浓度变化的曲线关系,并分析了主要因素对萃取的影响。通过再生萃取剂的循环萃取试验研究了其萃取效果,结果表明再生萃取剂可循环使用。

N掺杂石墨烯量子点的制备及在Fe^(3+)检测中的应用研究

研究了用热解柠檬酸制备发蓝光的石墨烯量子点(GQDs),并在此基础上,用(NH4)2CO3作N源,在水热条件下制备N掺杂石墨烯量子点(N-GQDs)。通过透射电子显微镜(TEM)、X射线光电子能谱仪(XPS)、傅里叶红外光谱仪(FT-IR)、紫外-可见吸收光谱仪(UV-Vis)、荧光光谱仪等对样品的结构和光学性能进行表征。此外,基于荧光淬灭原理,利用N-GQDs构建了一种检测Fe3+的荧光探针。研究表明,N-GQDs的荧光强度随Fe3+浓度的增大而降低,在0~60μmol/L范围内,N-GQDs荧光强度与Fe3+浓度有较好的线性关系,且该探针的检测限低达0.925μmol/L。

Fe^(3+)/g-C_3N_4光催化降解罗丹明B研究

罗丹明B是一种具有致癌、致突变等作用的难降解的工业污染物,如何高效地降解罗丹明B具有很重要的现实意义。本研究通过模板法和高温法配合制备Fe^(3+)/g-C_3N_4,采用X射线衍射分析、X射线光电子能谱、紫外-可见漫反射光谱等对其进行了表征,并以Fe^(3+)/g-C_3N_4为催化剂光催化降解罗丹明B。结果发现,该法成功制取了Fe^(3+)/g-C_3N_4,其对罗丹明B的降解效率较g-C_3N_4提高3.8倍,经过60min反应,98.3%罗丹明B被降解,说明Fe^(3+)/g-C_3N_4能有效地光催化降解罗丹明B,具有潜在的应用前景。

N503萃取Fe^(3+)等温线模型的建立与应用

分析N,N-二(1-甲庚基)乙酰胺(N503)萃取Fe3+的机理,并在结合软硬酸碱理论和萃酸等温线的基础上建立了N,N-二(1-甲庚基)乙酰胺萃取Fe3+的等温线模型,对模型进行实验验证.同时,运用界面吸附理论进一步阐述该模型的正确性.

沸石负载N、Fe^(3+)共掺杂TiO_2催化剂制备及表征

以人造沸石为载体,采用溶胶-凝胶法对N、Fe3+共掺杂TiO2进行负载化研究,探讨了焙烧温度、载体粒度、负载次数等因素对负载型光催化剂结构和催化活性的影响。研究了模拟太阳光下负载型光催化剂对活性染料SumifixTQ-Blue的降解性能,采用X射线衍射(XRD)、扫描电镜(SEM)和紫外—可见光漫反射吸收光谱(UV-VisDRS)等方法对催化剂进行了表征。结果表明,以60～80目人造沸石为载体,400℃下焙烧2h、负载3次的负载型光催化剂(N/Fe3+/TiO2-沸石催化剂)对SumifixTQ-Blue具有较高的降解率;N、Fe3+共掺杂发挥了两者的协同作用,增强了TiO2的紫外光吸收的同时也使其光吸收范围拓展到可见光区;而多孔材料沸石的引入也进一步提高了催化剂的催化活性。

Interconnected carbon nanocapsules with high N/S co-doping as stable and high-capacity potassium-ion battery anode

Carbonaceous materials have drawn much attention in potassium-ion batteries (PIBs) due to their low price and superior physicochemical properties. However, the application of carbonaceous materials in PIB anodes is hindered by sluggish kinetics and large volume expansion. Herein, N/S co-doped carbon nanocapsule (NSCN) is constructed for superior K+ storage. The NSCN possesses 3D nanocapsule framework with abundant meso/macropores, which guarantees structural robustness and accelerates ions/electrons transportation. The high-level N/S co-doping in carbon matrix not only generates ample defects and active sites for K+ adsorption, but also expands interlayer distance for facile K+ intercalation/deintercalation. As a result, the NSCN electrode delivers a high reversible capacity (408 mAh g^(−1) at 0.05 A g^(−1)), outstanding rate capability (149 mAh g^(−1) at 5 A g^(−1)) and favorable cycle stability (150m Ah g^(−1) at 2 A g^(−1) after 2000 cycles). Ex situ TEM, Raman and XPS measurements demonstrate the excellent stability and reversibility of NSCN electrode during potassiation/depotassiation process. This work provides inspiration for the optimization of energy storage materials by structure and doping engineering.

微波绿色合成N,S共掺杂碳点及其在Fe^(3+)检测和温度传感方面的应用

以韭菜为前驱体,采用微波法一步绿色合成N,S共掺杂的粒径均匀、分散性好的碳点。所合成的碳点近似球状,粒径2.0-5.0 nm。在365 nm的紫外灯照射下发明亮的蓝色荧光,发射峰具有激发波长依赖性。Fe^(3+)对所制备的碳点有明显选择性荧光猝灭现象。在5-300μmol/L的范围内,荧光猝灭程度(F/F_(0))与Fe^(3+)浓度呈现良好的线性关系(R=0.9930),检测限为4.0μmol/L。同时探测温度对制备碳点的影响,在20-55℃范围内,碳点荧光强度与温度具有较好的线性响应。由于生理温度范围在此温度范围内,所制备的碳点可用于细胞温度传感。

B,N,S共掺杂石墨烯量子点的制备及对Fe3+和H2PO4-的荧光检测

利用水热法制备了一种可在纯水体系中连续"OFF-ON-OFF"荧光识别Fe^3+和H2PO4^-的B,N,S共掺杂的石墨烯量子点探针材料(BNS-GQDs),并对其形貌和结构进行了表征,结果表明,BNS-GQDs粒径分布均匀,平均粒径为4nm,具有类似石墨烯的结构,且成功掺杂了B,N,S原子.光谱表征结果表明,其在纯水体系中可以实现对Fe^3+的荧光猝灭识别;同时,BNS-GQDs+Fe^3+体系能够专一性地荧光增强识别H2PO4^-.识别机理研究表明,BNS-GQDs可与Fe^3+通过静电作用形成配合物并向Fe^3+转移电子,从而引起荧光猝灭;H2PO4^-可从上述配合物中置换出Fe^3+,引起体系荧光恢复.BNS-GQDs识别Fe3+和H2PO4-具有较好的可逆性,可应用于Hela细胞和实际水样中Fe^3+和H2PO4^-的检测.

Hierarchical sulfur and nitrogen co-doped carbon nanocages as efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air battery

Exploring inexpensive and efficient bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) is critical for rechargeable metal-air batteries. Herein, we report a new 3D hierarchical sulfur and nitrogen co-doped carbon nanocages(hSNCNC) as a promising bifunctional oxygen electrocatalyst by an in-situ MgO template method with pyridine and thiophene as the mixed precursor. The as-prepared h SNCNC exhibits a positive half-wave potential of 0.792 V(vs. reversible hydrogen electrode, RHE) for ORR, and a low operating potential of 1.640 V at a 10 mA cm-2 current density for OER. The reversible oxygen electrode index is 0.847 V, far superior to commercial Pt/C and IrO2,which reaches the top level of the reported bifunctional catalysts. Consequently, the hSNCNC as air cathodes in an assembled Zn-air battery features low charge/discharge overpotential and long lifetime. The remarkable properties arises from the introduced multiple heteroatom dopants and stable 3D hierarchical structure with multi-scale pores, which provides the abundant uniform high-active S and N species and efficient charge transfer as well as mass transportation. These results demonstrate the potential strategy in developing suitable carbon-based bi-/multi-functional catalysts to enable the next generation of the rechargeable metal-air batteries.

A General Self-Sacrifice Template Strategy to 3D Heteroatom-Doped Macroporous Carbon for High-Performance Potassium-Ion Hybrid Capacitors

Potassium-ion hybrid capacitors(PIHCs)tactfully combining capacitor-type cathode with battery-type anode have recently attracted increasing attentions due to their advantages of decent energy density,high power density,and low cost;the mismatches of capacity and kinetics between capacitor-type cathode and battery-type anode in PIHCs yet hinder their overall performance output.Herein,based on prediction of density functional theory calculations,we find Se/N co-doped porous carbon is a promising candidate for K+storage and thus develop a simple and universal self-sacrifice template method to fabricate Se and N co-doped three-dimensional(3D)macroporous carbon(Se/N-3DMpC),which features favorable properties of connective hier-archical pores,expanded interlayer structure,and rich activity site for boosting pseudocapacitive activity and kinetics toward K^(+)storage anode and enhancing capacitance performance for the reversible anion adsorption/desorption cath-ode.As expected,the as-assembled PIHCs full cell with a working voltage as high as 4.0 V delivers a high energy density of 186 Wh kg^(−1) and a power output of 8100 W kg^(−1) as well as excellent long service life.The proof-of-concept PIHCs with excellent performance open a new avenue for the development and application of high-performance hybrid capacitors.

In Situ Preparation and Analysis of Bimetal Co?doped Mesoporous Graphitic Carbon Nitride with Enhanced Photocatalytic Activity

A novel photocatalyst of mesoporous graphitic carbon nitride(g-C_3N_4) co-doped with Co and Mo(Co/Mo-MCN) has been one-pot synthesized via a simple template-free method; cobalt chloride and molybdenum disulfide were used as the Co and Mo sources, respectively. The characterization results evidently indicate that molybdenum disulfide functions as Mo sources to incorporate Mo atoms in the framework of g-C_3N_4 and as a catalyst for promoting the decomposition of g-C_3N_4, resulting in the creation of mesopores. The obtained Co/Mo-MCN exhibited a significant enhancement of the photocatalytic activity in H_2 evolution(8.6 times) and Rhodamine B degradation(10.1 times) under visible light irradiation compared to pristine g-C_3N_4. Furthermore, density functional theory calculations were applied to further understand the photocatalytic enhancement mechanism of the optical absorption properties at the atomic level after Co-or Mo-doping. Finite-di erence time-domain simulations were performed to evaluate the e ect of the mesopore structures on the light absorption capability. The results revealed that both the bimetal doping and the mesoporous architectures resulted in an enhanced optical absorption; this phenomenon was considered to have played a critical role in the improvement in the photocatalytic performance of Co/Mo-MCN.

Fe^(3+)对同步硝化反硝化过程氮元素迁移转化及N_2O释放的影响

采用SBR反应器,研究了不同浓度的Fe3+对同步硝化反硝化(simultaneous nitrification denitrification,SND)过程中氮元素迁移转化去除和N2O释放的影响.结果表明,在同步硝化反硝化过程中,系统中Fe3+浓度为20 mg·L-1时可以提高系统对氮的去除率,而60 mg·L-1的Fe3+则会对其产生抑制效果.并且,高浓度的Fe3+会刺激SND过程中N2O的释放,N2O转化率也有所提高.这主要是因为:1高浓度的Fe3+会导致污泥脱氢酶活性降低,使得NO-2在好氧阶段大量累积;2高浓度的Fe3+减少了SND过程前置厌氧阶段胞内聚合物(polyhydroxybutyrate,PHB)的含量,使得后续反硝化过程碳源减少.Fe3+对SND过程中总磷的去除有促进作用,并且Fe3+浓度越高,总磷去除率越高,这主要是因为Fe3+的存在使系统中发生了化学除磷作用.

N和Fe^(3+)共掺杂TiO_2薄膜的制备及亲水性能研究

采用溶胶-凝胶法制备了N和Fe3+共掺杂的TiO2薄膜,研究了N,Fe3+不同掺杂比例、镀膜层数、热处理温度和光照时间等对TiO2薄膜亲水性能的影响.结果表明当掺杂物N和Fe3+的摩尔比为5.9∶1、镀膜层数为3层、热处理温度为550℃时,所制备的薄膜亲水性能最佳(接触角为2°).

Heterostructure design of Fe^(3)N alloy/porous carbon nanosheet composites for efficient microwave attenuation

The self-dissipation and attenuation capacity of materials play an important role in realizing efficient electromagnetic absorption,in this case,the roles of macroscopic composition and micro-structure should be emphasized simultaneously in the reasonable design of microwave absorbent.Given that,Fe_(3)N alloy embedded in two-dimensional porous carbon composites were fabricated via facile sol-gel and sacrificial template methods.Satisfactorily,the magnetic/dielectric materials combination and porous structure introduction are conductive to the optimization of impedance matching property,as result of the enhancement of microwave absorption capacity.In addition,sufficient magnetic loss capacity,strong conductivity as well as polarization attenuation bring about the outstanding microwave absorbing performance with an effective absorption bandwidth of 6.76 GHz and a minimum reflection loss value of-65.6 d B.It is believed that this work not only lay a foundation to achieve microwave response materials in a wide frequency range,but also emphasize the significant role of the component selection and structural design.

厌氧氨氧化颗粒污泥的培养及影响因素

在EGSB反应器中快速启动厌氧氨氧化(ANAMMOX)工艺,总氮去除速率为0.931±0.006 kg/(m^3·d),总氮去除效率为90.5%±0.8%。培养得到厌氧氨氧化颗粒污泥和絮状污泥混合物,污泥平均粒径为307.5μm。高质量浓度的NO_2^-(143.25 mg/L)抑制厌氧氨氧化菌活性;N_2H_4可强化厌氧氨氧化,但高质量浓度的N_2H_4抑制厌氧氨氧化菌活性;短期添加丙酸盐(COD质量浓度0~400 mg/L)对厌氧氨氧化速率几乎无影响;厌氧氨氧化速率随Fe^(3+)浓度(0~1.2 mmol/L)的增加而增加。

Fe^(3+)对不同进水氮磷比藻塘水质净化效果研究

铁是动植物进行生命活动不可缺少的元素。在藻塘内,铁能够影响藻细胞生长与繁殖,影响水质净化效果。通过研究不同浓度Fe3+对小球藻生长影响,并设定进水C/N和N/P,确定适宜Fe3+对藻塘出水理化性质及其污染物去除的影响。结果表明:当c(Fe3+)为10 000 nmol/L时,藻细胞质量增加约25%。适宜浓度Fe3+可调节藻塘水体DO、p H及ORP,提高净化效果。Fe3+利用率与COD、TN和TP去除率呈线性正相关,且随进水N/P的提高而增高。当ρ(N)/ρ(P)为50,ρ(C)/ρ(N)=5时,加铁藻塘COD、TN、TP去除率分别为45.34%、77.14%、43.11%,与未加铁藻塘相比,去除率分别提高约3,5.47,9.64个百分点。因此,铁可以促进藻类的生长,当藻塘进水ρ(C)∶ρ(N)∶ρ(P)∶ρ(Fe)为250∶50∶5∶1时,可降低污染物浓度,提高去除效果。

通过共掺杂策略优化氮化物电极的反应路径以促进碱性析氢反应动力学

通过优化氮化物的析氢反应(HER)途径来提高反应动力学是氮化物改性的重点.本工作创造性地采用P-阴离子和Ce-阳离子的共掺杂策略构建了P,Ce-FeNi_(3)N/NF电极.该P,Ce-FeNi_(3)N/NF电极在200 mV过电位下的电流密度(340 mA cm^(−2))是商业Pt/C@NF电流密度(174 mA cm^(−2))的两倍.理论计算表明,与FeNi_(3)N/NF的单个Ni活性位点不同,P,Ce-FeNi_(3)N/NF利用双活性位点(Ni和P)机制极大地优化了碱性HER过程中的反应动力学.此外,组装的NiFeCe-LDH/NF||P,Ce-FeNi_(3)N/NF电池仅需要1.537 V的电压即可实现500 mA cm^(−2)的高电流密度.这项工作从反应路径优化和反应动力学改进的角度为实现氮化物优异的电催化性能提供了一种新策略.