构筑Bi纳米粒子负载BiOCl纳米片欧姆结用于光催化CO_(2)还原

煤炭、石油和天然气等能源的不断增长消耗,不仅导致不可再生能源逐渐枯竭,还使大气中的CO_(2)浓度显著上升,引发严重的能源危机和气候问题。因此,我们必须开发清洁、可持续的能源转换技术,以应对不断增长的能源需求和日益严重的环境危机。受到自然界光合作用的启发,光催化CO_(2)转化利用太阳能驱动,可以将CO_(2)和水转化为高附加值的化学品。经过多年的发展,人工光合作用已被认为是一种绿色、经济、可持续的方法,有望助力实现国家的碳中和发展目标。然而,现有的光催化剂存在着载流子分离效率低和活性位点不足的问题,从而导致CO_(2)光还原效率较低。为了应对这些科学问题,研究人员发现将金属纳米粒子负载到半导体材料上形成欧姆结,可以产生内建电场,有助于光生电子和空穴的分离。因此,本研究通过溶剂热法在BiOCl纳米片表面负载Bi纳米粒子,构建了Bi/BiOCl欧姆结光催化剂。通过X射线衍射(XRD)、X射线光电子能谱(XPS)和透射电子显微镜(TEM)分析了光催化剂的成分和微观结构。利用紫外-可见漫反射光谱(UV-Vis DRS)研究了催化剂的光吸收性能。通过瞬态光电流响应测试、电化学阻抗谱(EIS)和电子自旋共振谱(ESR)研究了光生电子和空穴的分离能力。由于Bi纳米粒子与BiOCl的功函数不同,二者形成的欧姆结具有优异的电荷转移特性,可以显著提高光生载流子的利用效率。此外,Bi纳米粒子还可以作为助催化剂,促进惰性CO_(2)分子的活化。光催化测试结果显示,经过300 W氙灯照射4 h后,具有最佳活性的复合材料(Bi/BiOCl-2)将CO_(2)还原为CO(34.31μmol·g^(-1))和CH_(4)(1.57μmol·g^(-1))的速率分别是BiOCl纳米片的2.55倍和4.76倍。同位素示踪实验证实,产物是CO_(2)和水分子经过光催化反应得到的。此外,根据原位傅里叶变换红外光谱(in situ FTIR)结果,发现在CO_(2)还原过程中形成了^(*)CHO、^(*)CH_(3)O、b-CO_(3)^(2-)、m-CO_(3)^(2-)、HCO_(3)^(-)、HCOOH、^(*)COOH和HCOO^(-)等中间体,并进一步提出了可能的光催化CO_(2)还原机制。经过25 h的CO_(2)光还,原反应后,CO和CH_(4)产量持续增加,同时结合XRD、XPS和TEM结果表明,制备的Bi/BiOCl-2材料具有良好的结构稳定性。这项研究为高效CO_(2)光还原催化剂的构建提供了有益的参考。

Phosphotungstic acid ionic liquid for efficient photocatalytic desulfurization:Synthesis,application and mechanism

An efficient mass transfer process is a critical factor for regulating catalytic activity in a photocatalytic desulfurization system.Herein,a phosphotungstic acid(HPW)active center is successfully composited with a quaternary ammonium phosphotungstate-based hexadecyltrimethylammonium chloride ionic liquid(CTAC-HPW)by the ion exchange method for the photocatalytic oxidative desulfurization of dibenzothiophene sulfide.The keggin structure of HPW and highly mass transfer performance of organic cations synergistically enhanced the photocatalytic activity towards the effective convertion of dibenzothiophene(DBT)with the excitation of visible light.The deep desulfurization(<10 mg·kg^(-1))is attained within 30 min,and well stability is demonstrated within 25 cycles.Moreover,the CTAC-HPW photocatalyst projects well selectivity to interference from coexisting compounds such as olefins and aromatic hydrocarbons and universality of dibenzothiophenes,for example,4-methyldibenzothiophene(4-MDBT)and 4,6-dimethyldibenzothiophene(4,6-DMDBT).Ultimately,a possible photocatalytic desulfurization mechanism is proposed according to the Gaschromatography-mass spectrometry(GC-MS),proving that the final product is the corresponding sulfone.The trapping experiment and electron spin resonance(ESR)analysis confirmed that h^(+)and,COOH played critical roles in the oxidation process.The work offers a practicable strategy for efficiently converting DBT to DBTO_(2) with added value.

Multifunctional AlPO_(4)reconstructed LiMn_(2)O_(4)surface for electrochemical lithium extraction from brine

LiMn_(2)O_(4)(LMO)electrochemical lithium-ion pump has gained widespread attention due to its green,high efficiency,and low energy consumption in selectively extracting lithium from brine.However,collapse of crystal structure and loss of lithium extraction capacity caused by Mn dissolution loss limits its industrialized application.Hence,a multifunctional coating was developed by depositing amorphous AlPO_(4)on the surface of LMO using sol-gel method.The characterization and electrochemical performance test provided insights into the mechanism of Li^(+)embedment and de-embedment and revealed that multifunctional AlPO_(4)can reconstruct the physical and chemical state of LMO surface to improve the interface hydrophilicity,promote the transport of Li^(+),strengthen cycle stability.Remarkably,after 20 cycles,the capacity retention rate of 0.5AP-LMO reached 93.6%with only 0.147%Mn dissolution loss.The average Li^(+)release capacity of 0.5AP-LMO//Ag system in simulated brine is 28.77 mg/(g h),which is 90.4%higher than LMO.Encouragingly,even in the more complex Zabuye real brine,0.5AP-LMO//Ag can still maintain excellent lithium extraction performance.These results indicate that the 0.5AP-LMO//Ag lithium-ion pump shows promising potential as a Li^(+)selective extraction system.

Few-layered hexagonal boron nitride nanosheets stabilized Pt NPs for oxidation promoted adsorptive desulfurization of fuel oil

A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structure and the defective sites of h-BNNS not only are beneficial to the stabilization of Pt NPs but also favor the adsorption of aromatic sulfides.By employing Pt/h-BNNS with a Pt loading amount of 1.19 wt%as the active adsorbent and air as an oxidant,a 98.0%sulfur removal over dibenzothiophene(DBT)is achieved along with a total conversion of the DBT to the corresponding sulfones(DBTO_(2)).Detailed experiments show that the excellent desulfurization activity originates from the few-layered structure of h-BNNS and the high catalytic activity of Pt NPs.In addition,the OPADS system with Pt/h-BNNS as the active adsorbent shows remarkable stability in desulfurization performance with the existence of different interferents such as olefin,and aromatic hydrocarbons.Besides,the Pt/h-BNNS can be recycled 12 times without a significant decrease in desulfurization performance.Also,a process flow diagram is proposed for deep desulfurization of fuel oil and recovery of high value-added products,which would promote the industrial application of such OPADS strategy.

磁性可循环高熵金属氧化物催化剂用于活化氧气催化氧化脱硫

燃油中的含硫化合物燃烧会导致酸雨、雾霾等环境问题,因此需要降低燃油中硫化物浓度.但是,目前工业上采用的加氢脱硫(HDS)技术在脱除芳香硫化物时需要更高的温度、压力和氢耗,不利于碳减排(生产1吨H2排放10–20吨CO_(2)),因此亟需开发非HDS工艺.在各种非HDS技术中,以O_(2)为氧化剂的氧化脱硫(ODS)技术由于具有对芳香族硫化物脱除性能高、成本低、反应条件温和等优点,而受到广泛关注.在ODS过程中,催化剂的设计是关键之一.研究发现,金属氧化物具有较好的活化O_(2)性能,但是传统金属氧化物存在活性位点有限、分离回收较难等不足.近年来,人们发现,高熵金属氧化物在以O_(2)为氧化剂的催化氧化反应中表现出较好的催化性能,但如何进一步提升其循环使用性能,是目前高熵金属氧化物在ODS中应用所面临的挑战.为解决上述问题,本文通过组分设计在高熵金属氧化物催化剂中引入高催化活性组分和磁性元素,再采用机械化学球磨辅助高温煅烧策略,构筑了一类新型磁性高熵金属氧化物催化剂(CoCrFeMnNiO_(x),HEMO),并用于活化O_(2)催化氧化脱除燃油中芳香族硫化物.实验发现,900℃煅烧制得的HEMO-900催化剂性能最优.催化剂的结构表征结果表明,通过球磨辅助策略能够降低高熵结构的形成温度.进一步研究表明,高熵结构不仅能够提升催化活性组分的分散度,而且有助于活性组分的电荷调控,从而显著增强了HEMO-900对O_(2)分子的活化能力.将所制备的HEMO-900催化剂用于以O_(2)为氧化剂的燃油氧化脱硫体系中,能够获得较好的脱硫性能,在最优条件下能够获得96.9%的脱硫率(硫化物浓度降低至0.001%以下).此外,HEMO-900催化剂能够高效氧化脱除燃油中不同种类芳香族硫化合物,拓宽了其在不同类型燃油深度脱硫中的应用.进一步分析发现,HEMO-900催化剂可以将燃油中二苯并噻吩定向氧化为二苯并噻吩砜.同时,HEMO-900催化剂对真实油品中的硫化物也表现出较好的脱除性能.此外,HEMO-900催化剂还有较好的磁性循环使用性能:通过外加磁场,可以快速将HEMO-900催化剂与燃油相分离,该性能使得催化剂能够在连续反应过程中被高效回收和重复利用.本研究中,HEMO-900催化剂在5次循环使用后,其ODS活性仍达到91.1%综上所述,本文通过机械化学球磨辅助高温煅烧法成功合成了一种可磁性回收的高熵金属氧化物催化剂,实验发现了机械球磨辅助能够显著降低高熵结构的形成温度.设计制得的催化剂兼具较好的活化O_(2)催化燃油氧化脱硫性能和可磁性分离回收的特点.通过设计该类可磁性分离的高熵金属氧化物催化剂,不仅为实现温和条件下燃油深度脱硫提供新的选择,而且为其他多相催化氧化反应催化剂设计提供了新思路.

One-pot in-situ synthesis of coralloid supported VO_(2)catalyst for intensified aerobic oxidative desulfurization

A coralloid 3D g-C_(3)N_(4)supported VO_(2)catalyst was successfully synthesized in-situ by one-pot method,avoiding the agglomeration of VO_(2)during the reaction.The morphological and compositional information of the supported catalyst were investigated detailedly.30%VO_(2)/3D g-C_(3)N_(4)revealed excellent catalytic activity in aerobic oxidative desulfurization,the oxidative of dibenzothiophene(DBT),4-methyldibenzothiophene(4-MDBT)and 4,6-dimethyldibenzothiophene(4,6-DMDBT)reached 98.6%,99%and 99.4%,respectively,under the same mild conditions.The recycling performance and the mechanism on the oxidative of DBT were studied as well.

Construction of truncated-octahedral LiMn2O4 for battery-like electrochemical lithium recovery from brine

The extraction of lithium from salt lakes or seawater has attracted worldwide attention because of the explosive growth of global demand for lithium products. The LiMn_(2)O_(4)-based electrochemical lithium recovery system is one of the strongest candidates for commercial application due to its high inserted capacity and low energy consumption. However, the surface orientation of LiMn_(2)O_(4)that facilitates Li diffusion happens to be prone to manganese dissolution making it a great challenge to obtain high lithium inserted capacity and long life simultaneously. Herein, we address this problem by designing a truncated octahedral LiMn_(2)O_(4)(Tr-oh LMO) in which the dominant(111) facets minimize Mn dissolution while a small portion of(100) facets facilitate the Li diffusion. Thus, this Tr-oh LMO-based electrochemical lithium recovery system shows excellent Li recovery performance with high inserted capacity(20.25 mg g^(-1)per cycle) in simulated brine. In addition, the dissolution rate of manganese per 30 cycles is only 0.44% and the capacity maintained 85% of the initial after 30 cycles. These promising findings accelerate the practical application of LiMn_(2)O_(4)in electrochemical lithium recovery.

Construction of porous disc-like lithium manganate for rapid and selective electrochemical lithium extraction from brine

In order to satisfy the growing global demand for lithium, selective extraction of lithium from brine has attracted extensive attention. LiMn_(2)O_(4)-based electrochemical lithium recovery system is one of the best choices for commercial applications because of its high selectivity and low energy consumption.However, the low ion diffusion coefficient of lithium manganate limits the further development of electrochemical lithium recovery system. In this work, a novel porous disc-like LiMn_(2)O_(4) was successfully synthesized for the first time via two-step annealing manganese(Ⅱ) precursors. The as-prepared LiMn_(2)O_(4) exhibits porous disc-like morphology, excellent crystallinity, high Li^(+)diffusion coefficient(average 7.6×10^(-9)cm^(2)·s^(-1)), high cycle stability(after 30 uninterrupted extraction and release cycles, the crystal structure hardly changed) and superior rate capacity(93.5% retention from 10-120 mA·g^(-1)). The porous structure and disc-like morphology further promote the contact between lithium ions and electrode materials. Therefore, the assembled electrochemical lithium extraction device with LiMn_(2)O_(4) as positive electrode and silver as negative electrode can realize the rapid and selective extraction of lithium in simulated brine(adsorption capacity of lithium can reach 4.85 mg·g^(-1) in 1 h). The mechanism of disc-like LiMn_(2)O_(4) in electrochemical lithium extraction was proposed based on the analysis of electrochemical characterization and quasi in situ XRD. This novel structure may further promote the practical application of electrochemical lithium extraction from brine.

Cu^2+改性g-C3N4光催化剂的光催化性能

本文通过将Cu^2+掺入g-C3N4结构中成功制备了Cu/g-C3N4光催化剂,并进一步优化其光催化性能。同时,采用多种表征方法对Cu/g-C3N4光催化剂的结构、形貌、光学和光电性能进行了分析。X射线衍射(XRD)和X射线光电子能谱(XPS)结果表明制备的光催化剂为Cu/g-C3N4,且Cu的价态为+2。在可见光照射下,研究了不同铜含量的Cu/g-C3N4和gC3N4光催化剂的光催化活性。实验结果表明,Cu/g-C3N4光催化剂的降解能力显著高于纯相的g-C3N4。N2吸附-解吸等温线表明,Cu^2+的引入对g-C3N4的微观结构影响不大,说明光催化活性的提高可能与光生载流子的有效分离有关。因此,Cu/g-C3N4光催化降解RhB和CIP性能的提升可能是由于Cu^2+可以作为电子捕获陷阱从而降低了载流子的复合速率。通过光电测试表明,在g-C3N4中掺入Cu^2+可以降低g-C3N4的电子空穴复合速率,加速电子空穴对的分离,从而提高了其光催化活性。自由基捕获实验和电子自旋共振(ESR)结果表明,超氧自由基(O2·-)、羟基自由基(·OH)和空穴的协同作用提高了Cu/g-C3N4光催化剂的光催化活性。

Pt nanoparticles encapsulated on V_(2)O_(5)nanosheets carriers as efficient catalysts for promoted aerobic oxidative desulfurization performance

Platinum group metals(PGMs)usually exhibit promising aerobic catalytic abilities,providing a green and feasible oxidative desulfurization method.However,often,the PGM nanoparticles(NPs)get leached,and the catalysts are deactivated.In this work,Pt NPs with particle sizes of approximately 4–5 nm were encapsulated effectively and uniformly on the surface of vanadium pentoxide(V2O5)nanosheets(with thicknesses of approximately six atomic layers)through strong metal-support interactions.The synthesized catalysts promote catalytic aerobic oxidation reactions,realizing deep desulfurization(99.1%,<5μg g^(–1))under atmospheric pressure and 110℃reaction temperature.Remarkable degrees of sulfur removal could be achieved for oils with different initial S-concentrations and substrates.Additionally,the as-prepared catalysts could be recycled for reuse at least seven times.

Progress in electrochemical lithium ion pumping for lithium recovery

Accelerating the development of lithium resources has attracted a great deal of attention with the explosive growth of new energy vehicles.As a new technology,electrochemical lithium ion pumping(ELIP)is featured by environment-friendly,low energy consumption and high efficiency.This review summarizes the research progress in ELIP,and focuses on the evaluation methods,electrode materials and electrochemical systems of ELIP.It can be concluded that ELIP is expected to achieve an industrial application and has a promising prospect.In addition,challenges and perspective of electrochemical lithium extraction are also highlighted.

Hexagonal boron nitride adsorbent: Synthesis, performance tailoring and applications

Hexagonal boron nitride(h-BN),with unique structural and properties,has shown enormous potentitoward variety of possible applications.By virtue of partially-ionic character of BN chemical bonds anusually large specific surface area,h-BN-related nanostructures exhibit appealing adsorption propertiewhich can be widely applied for separation and purification towards energy and environment treatmenIn this review,recent progress in designing h-BN micro,nano-structure,controlled synthesis,performancoptimizing as well as energy and environment-related adsorption applications are summarized.Strategieto tailor the h-BN can be classified as morphology control,element doping,defect control and surfacmodification,focusing on how to optimize the adsorption performance.In order to insight the intrinsimechanism of tuning strategies for property optimization,the significant adsorption applications of h-Btowards hydrogen storage,CO2 capture,pollutants removal from water and adsorption desulfurization arpresented.

Catalytic oxidative desulfurization of fuels in acidic deep eutectic solvents with [(C_6H_(13))_3P(C_(14)H_(29))]_3PMo_(12)O_(40) as a catalyst

Deep eutectic solvents(DESs) are a new class of green solvents analogous to ionic liquids due to their biodegradable capacity and low cost. However, the direct extractive desulfurization of diesel oil by DESs cannot meet the government’s standard. In this work, amphiphilic polyoxometalates were synthesized and characterized by FT-IR and mass spectrometry.The oxidative desulfurization results showed that benzothiophene(BT) could be completely removed by employing a [(CH)P(CH)]PMoO, DES(ChCl/2 Ac) and HOsystem. It was also found that the organic cation of catalysts played a positive role in oxidative desulfurization. The reaction conditions, such as reaction temperature and time, the amount of catalyst and DES and HO/S(O/S) molar ratio, were optimized. Different sulfides were tested to determine the desulfurization selectivity of the optimal reaction system, and it was found that 97.2% of dibenzothiophene(DBT) could be removed followed by 80.7% of 4-MDBT and 76.0% of 4,6-DMDBT. After reaction, the IR spectra showed that the catalyst [(CH)P(CH)]PMoOwas stable during the reaction process and the oxidative product was dibenzothiophene sulfone(DBTO). Furthermore, the catalyst can be regenerated and recycled for four runs with little loss of activity.

Hexagonal boron nitride:A metal-free catalyst for deep oxidative desulfurization of fuel oils

Oxidative desulfurization(ODS)has been proved to be an efficient strategy for the production of clean fuel oil.Numerous metal-based materials have been employed as excellent ODS catalysts,but being hindered by their high-cost and potential secondary pollution.In this work,we employed graphene analogous hexagonal boron nitride(h-BN)as a metal-free catalyst for ODS with hydrogen peroxide(H2O2)as the oxidant.The h-BN catalyst was characterized and proved to be a few-layered structure with relatively high specific surface areas.The h-BN catalyst showed a 99.4%of sulfur removal in fuel oil under the optimized reaction conditions.Besides,the h-BN can be recycled for 8 times without significant decrease in the catalytic performance.Detailed mechanism analysis found that it is the boron radicals in h-BN activated H2O2 to generate·OH species,which can readily oxidize sulfides to corresponding sulfones for separation.This work would provide another choice in choosing metal-free catalysts for ODS.

Boosting photocatalytic degradation of RhB via interfacial electronic effects between Fe-based ionic liquid and g-C_3N_4

The Fe-based ionic liquid doped g-C_3N_4(Fee CN) photocatalyst was firstly prepared base on ultrathin g-C_3N_4 obtained by multiple calcination method with a metal-based reactive ionic liquid [Omim]FeCl_4 for the degradation of Rhodamine B(RhB). Experimental results revealed that Fe3+species were doped into the framework of g-C_3N_4. The effect of the amount of Fe-doping on the catalytic activity was performed. The result showed that the Fee CN could effectively degrade RhB under the condition of visible light irradiation. The photocurrent analysis showed that the incorporation of Fe^(3+)into g-C_3N_4 material could accelerate the separation of the photogenerated carriers significantly.At the same time, the reactive species generated during the photodegradation process were tested by radicals trapping experiments and electron spin resonance(ESR). It was proposed that the synergistic effect of■ and ·OH contributed to degrade RhB efficiently.

Scalable and facile synthesis of V_(2)O_(5) nanoparticles via ball milling for improved aerobic oxidative desulfurization

In recent years, transition-metal oxides(TMOs) have been long employed for aerobic oxidative desulfurization. However, the inherent bottlenecks, such as the low explosion of active sites, limit the application of bulk TMOs catalyst. In this study, V_(2)O_(5) nanoparticles with oxygen vacancies were prepared in large-scale via facile ball milling strategy with adding oxalic acid as a reducing agent. The as-prepared catalysts exhibit remarkable sulfur removal for oils with different initial S-concentrations and different substrates. Sulfur removal could reach up to 99.7%(< 2 ppm) under the optimized reaction conditions. This work provides a feasible desulfurization strategy for fuel oils.

Polyoxometalate-based silica-supported ionic liquids for heterogeneous oxidative desulfurization in fuels

With the aim of deep desulfurization, silica-supported polyoxometalate-based ionic liquids were successfully prepared by a one-pot hydrothermal process and employed in heterogeneous oxidative desulfurization of various sulfur compounds. The compositions and structures of the hybrid samples were characterized by various methods such as FT-IR, XPS, Raman,UV–Vis, wide-angle XRD and N2adsorption–desorption. The experimental results indicated that the hybrid materials presented a high dispersion of tungsten species and excellent catalytic activity for the removal of 4,6-dimethyldibenzothiophene without any organic solvent as extractant, and the sulfur removal could reach 100.0% under mild conditions.The catalytic performance on various substrates was also investigated in detail. After cycling seven cycles, the sulfur removal of the heterogeneous system still reached 93.0%. The GC-MS analysis results demonstrated that the sulfur compound was first adsorbed by the catalyst and subsequently oxidized to its corresponding sulfone.

3D-printing of integrated spheres as a superior support of phosphotungstic acid for deep oxidative desulfurization of fuel

Construction of catalysts with integral structure for oxidative reaction process is an essential promotion to catalysts in industrial application.In this work,a 3D printing method was employed to prepare 3D printed spheres(3D-PSs),followed by carbonization to form 3D carbon spheres(3D-CSs).Then,a 3D-CSs supported phosphotungstic acid(HPW/3D-CSs)was prepared for deep oxidative desulfurization.Compared with traditional powder catalysts,the as-prepared catalyst is easy to be operated and separated from oil products.The supported catalyst possesses excellent catalytic performance and the removal of DBT,4-MDBT and 4,6-DMDBT in fuel oil,reaching^100%of sulfur removal.The effects of various experimental parameters on desulfurization efficiency were considered to optimize reaction conditions.Moreover,the catalyst shows excellent thermal and chemical stability,with no obvious decrease in desulfurization activity after 5 cycles.GC–MS analysis indicates DBT sulfone was the solely oxidized product of DBT.

Electrochemical lithium ions pump for lithium recovery from brine by using a surface stability Al_(2)O_(3)–ZrO_(2 )coated LiMn_(2)O_(4) electrode

The rapid commercialization of lithium–ion batteries has caused significant expansion of the lithium demand.Electrochemical lithium ions pump is a promising technology because of its good selectivity and friendly environment.Herein,an Al_(2)O_(3)–ZrO_(2) film coating of the LiMn_(2)O_(4)(AlZr–LMO) electrode is prepared and operated for recovery of Li^(+)from brine.The Li^(+) maximum extraction capacity of AlZr–LMO reached 49.92 mg/g in one cycle.Compared with the solely LMO electrode,the AlZr–LMO demonstrated evident electrochemical stability and cycle life towards the Li^(+)recovery system.After 30 successive cycles,the extraction capacity for Li^(+)increased from 29.21%to 57.67%.The high cycle capacity of the material could be attributed to its low polarization,high active sites,and good chemical stability of the electrode surface owing to the synergy function of Al_(2)O_(3)–ZrO_(2)in the charging-discharging process.A dynamic model parameter identification method was performed to evaluate the active site of AlZr–LMO.This work may provide a way to design the AlZr–LMO electrode and develop a good method for the recovery of lithium from brine.

Amorphous TiO_2-supported Keggin-type ionic liquid catalyst catalytic oxidation of dibenzothiophene in diesel

Supported ionic liquid(IL) catalysts [Cmim]PMoO/Am TiO(amorphous TiO) were synthesized through a one-step method for extraction coupled catalytic oxidative desulfurization(ECODS) system. Characterizations such as FTIR, DRS,wide-angle XRD, Nadsorption–desorption and XPS were applied to analyze the morphology and Keggin structure of the catalysts. In ECODS with hydrogen peroxide as the oxidant, it was found that ILs with longer alkyl chains in the cationic moiety had a better effect on the removal of dibenzothiophene. The desulfurization could reach 100% under optimal conditions, and GC–MS analysis was employed to detect the oxidized product after the reaction. Factors affecting the desulfurization efficiencies were discussed, and a possible mechanism was proposed. In addition, cyclic experiments were also conducted to investigate the recyclability of the supported catalyst. The catalytic activity of [Cmim]PMoO/Am TiOonly dropped from 100% to 92.9% after ten cycles, demonstrating the good recycling performance of the catalyst and its potential industrial application.