PDF(1984 KB)
双氧原子掺杂的氮化硼材料用于吸附脱硫研究
Jing Luo, Yanchen Wei, Yanhong Chao, Chao Wang, Hongping Li, Jun Xiong, Mingqing Hua, Huaming Li, Wenshuai Zhu
工程（英文） ›› 2022, Vol. 14 ›› Issue (7) : 86-93.
PDF(1984 KB)
PDF(1984 KB)
双氧原子掺杂的氮化硼材料用于吸附脱硫研究
Engineering Dual Oxygen Simultaneously Modified Boron Nitride for Boosting Adsorptive Desulfurization of Fuel
氧原子普遍共存于六方氮化硼（h-BN）吸附剂中。如何利用h-BN中的氧原子以强化其与吸附质之间的相互作用，从而提高材料的吸附性能，是一个亟待解决课题。本文以聚合法构建氧原子晶格内部取代和边缘羟基化修饰的双氧原子位点改性BN（BN‒2O）材料。BN‒2O的边缘羟基氧原子能够增强二苯并噻吩（DBT）与其非均匀表面的π-π作用，从而促进多分子层型吸附过程。实验结果表明，相比边缘羟基取代BN（BN‒OH）材料，BN‒2O材料对燃油中DBT的吸附容量提升了12%。密度泛函理论计算还揭示了BN‒2O晶格内部的氧原子可以通过极化吸附质的方式增强其与BN‒2O之间的偶极作用，进一步提高BN‒2O从富含芳烃的燃油中选择性吸附DBT的能力，使得其在燃油吸附脱硫领域表现出更好的应用前景。吸附结果符合Freundlich模型和准二级动力学模型结果。因此，该聚合法同样可被应用于其他杂原子掺杂体系以提升吸附剂的吸附性能。
Oxygen atoms usually co-exist in the lattice of hexagonal boron nitride (h-BN). The understanding of interactions between the oxygen atoms and the adsorbate, however, is still ambiguous on improving adsorptive desulfurization performance. Herein, simultaneously oxygen atom-scale interior substitution and edge hydroxylation in BN structure were constructed via a polymer-based synthetic strategy. Experimental results indicated that the dual oxygen modified BN (BN–2O) exhibited an impressively increased adsorptive capacity about 12% higher than that of the edge hydroxylated BN (BN–OH) fabricated via a traditional method. The dibenzothiophene (DBT) was investigated to undergo multi-molecular layer type coverage on the BN–2O uneven surface via π–π interaction, which was enhanced by the increased oxygen doping at the edges of BN–2O. The density functional theory calculations also unveiled that the oxygen atoms confined in BN interior structure could polarize the adsorbate, thereby resulting in a dipole interaction between the adsorbate and BN–2O. This effect endowed BN–2O with the ability to selectively adsorb DBT from the aromatic-rich fuel, thereafter leading to an impressive prospect for the adsorptive desulfurization performance of the fuel. The adsorptive result was in good accordance with Freundlich and pseudo-second-order adsorption kinetics model results. Therefore, the designing of a polymer-based strategy could be also extended to other heteroatom doping systems to enhance adsorptive performance.
聚合物基合成策略 / 内部取代BN / 氧掺杂 / 吸附脱硫
Polymer-based synthetic strategy / Interior substitution BN / Oxygen doping / Adsorptive desulfurization
| [1] |
Laredo GC, Vega Merino PMV, Hernández PS. Light cycle oil upgrading to high quality fuels and petrochemicals: a review. Ind Eng Chem Res 2018;57 (22):7315–21.
|
| [2] |
Cao Z, Zhang X, Xu C, Huang X, Wu Z, Peng C, et al. Selective hydrocracking of light cycle oil into high-octane gasoline over bi-functional catalysts. J Energy Chem 2021;52:41–50.
|
| [3] |
Yang C, Li R, Cui C, Liu S, Qiu Q, Ding Y, et al. Catalytic hydroprocessing of microalgae-derived biofuels: a review. Green Chem 2016;18(13):3684–99.
|
| [4] |
Stanislaus A, Marafi A, Rana MS. Recent advances in the science and technology of ultra low sulfur diesel (ULSD) production. Catal Today 2010;153(1–2):1–68.
|
| [5] |
Zhang M, Liu J, Yang J, Chen X, Wang M, Li H, et al. Molybdenum-containing dendritic mesoporous silica spheres for fast oxidative desulfurization in fuel. Inorg Chem Front 2019;6(2):451–8.
|
| [6] |
Wang C, Qiu Y, Wu HY, Yang WS, Zhu Q, Chen ZG, et al. Construction of 2D–2D V2O5/BNNS nanocomposites for improved aerobic oxidative desulfurization performance. Fuel 2020;270:117498.
|
| [7] |
Zhu W, Wang C, Li H, Wu P, Xun S, Jiang W, et al. One-pot extraction combined with metal-free photochemical aerobic oxidative desulfurization in deep eutectic solvent. Green Chem 2015;17(4):2464–72.
|
| [8] |
Jiang W, Jia H, Li H, Zhu L, Tao R, Zhu W, et al. Boric acid-based ternary deep eutectic solvent for extraction and oxidative desulfurization of diesel fuel. Green Chem 2019;21(11):3074–80.
|
| [9] |
Jiang W, Zhu K, Li HP, Zhu LH, Hua MQ, Xiao J, et al. Synergistic effect of dual Brønsted acidic deep eutectic solvents for oxidative desulfurization of diesel fuel. Chem Eng J 2020;394:124831.
|
| [10] |
Bhadra BN, Jhung SH. Well-dispersed Ni or MnO nanoparticles on mesoporous carbons: preparation via carbonization of bimetallic MOF-74s for highly reactive redox catalysts. Nanoscale 2018;10(31):15035–47.
|
| [11] |
Almashjary KH, Khalid M, Dharaskar S, Jagadish P, Walvekar R, Gupta TCSM. Optimisation of extractive desulfurization using choline chloride-based deep eutectic solvents. Fuel 2018;234:1388–400.
|
| [12] |
Wagle DV, Zhao H, Deakyne CA, Baker GA. Quantum chemical evaluation of deep eutectic solvents for the extractive desulfurization of fuel. ACS Sustain Chem Eng 2018;6(6):7525–31.
|
| [13] |
Iravani AA, Gunda K, Ng FTT. Adsorptive removal of refractory sulfur compounds by tantalum oxide modified activated carbons. AIChE J 2017;63 (11):5044–53.
|
| [14] |
Ren X, Liu Z, Dong L, Miao G, Liao N, Li Z, et al. Dynamic catalytic adsorptive desulfurization of real diesel over ultra-stable and low-cost silica gelsupported TiO2. AIChE J 2018;64(6):2146–59.
|
| [15] |
Han Y, Sinnwell MA, Teat SJ, Sushko ML, Bowden ME, Miller QRS, et al. Desulfurization efficiency preserved in a heterometallic MOF: synthesis and thermodynamically controlled phase transition. Adv Sci 2019;6 (7):1802056.
|
| [16] |
Khan NA, An HJ, Yoo DK, Jhung SH. Polyaniline-derived porous carbons: remarkable adsorbent for removal of various hazardous organics from both aqueous and non-aqueous media. J Hazard Mater 2018;360:163–71.
|
| [17] |
Sarker M, An HJ, Yoo DK, Jhung SH. Nitrogen-doped porous carbon from ionic liquid@Al–metal–organic framework: a prominent adsorbent for purification of both aqueous and non-aqueous solutions. Chem Eng J 2018;338:107–16.
|
| [18] |
Qin JX, Tan P, Jiang Y, Liu XQ, He QX, Sun LB. Functionalization of metal– organic frameworks with cuprous sites using vapor-induced selective reduction: efficient adsorbents for deep desulfurization. Green Chem 2016;18(11):3210–5.
|
| [19] |
Zhu W, Wu Z, Foo GS, Gao X, Zhou M, Liu B, et al. Taming interfacial electronic properties of platinum nanoparticles on vacancy-abundant boron nitride nanosheets for enhanced catalysis. Nat Commun 2017;8(1):15291.
|
| [20] |
Zhu W, Gao X, Li Q, Li H, Chao Y, Li M, et al. Controlled gas exfoliation of boron nitride into few-layered nanosheets. Angew Chem Int Ed 2016;55 (36):10766–70.
|
| [21] |
Chao YH, Pang JY, Bai Y, Wu PW, Luo J, He J, et al. Graphene-like BN@SiO2 nanocomposites as efficient sorbents for solid-phase extraction of rhodamine B and rhodamine 6G from food samples. Food Chem 2020;320:126666.
|
| [22] |
Pakdel A, Bando Y, Golberg D. Nano boron nitride flatland. Chem Soc Rev 2014;43(3):934–59.
|
| [23] |
Lu L, He J, Wu P, Wu Y, Chao Y, Li H, et al. Taming electronic properties of boron nitride nanosheets as metal-free catalysts for aerobic oxidative desulfurization of fuels. Green Chem 2018;20(19):4453–60.
|
| [24] |
Wu P, Zhu W, Chao Y, Zhang J, Zhang P, Zhu H, et al. A template-free solventmediated synthesis of high surface area boron nitride nanosheets for aerobic oxidative desulfurization. Chem Commun 2016;52(1):144–7.
|
| [25] |
Ling Z, Wang Z, Zhang M, Yu C, Wang G, Dong Y, et al. Sustainable synthesis and assembly of biomass-derived B/N Co-doped carbon nanosheets with ultrahigh aspect ratio for high-performance supercapacitors. Adv Funct Mater 2016;26(1):111–9.
|
| [26] |
Chen S, Chen Z, Siahrostami S, Higgins D, Nordlund D, Sokaras D, et al. Designing boron nitride islands in carbon materials for efficient electrochemical synthesis of hydrogen peroxide. J Am Chem Soc 2018;140 (25):7851–9.
|
| [27] |
Pang J, Chao Y, Chang H, Li H, Xiong J, Zhang Q, et al. Silver nanoparticledecorated boron nitride with tunable electronic properties for enhancement of adsorption performance. ACS Sustain Chem Eng 2018;6(4):4948–57.
|
| [28] |
Chao YH, Zhang J, Li HP, Wu PW, Li XW, Chang HH, et al. Synthesis of boron nitride nanosheets with N-defects for efficient tetracycline antibiotics adsorptive removal. Chem Eng J 2020;387:124138.
|
| [29] |
Xiong J, Zhu WS, Li HP, Yang L, Chao YH, Wu PW, et al. Carbon-doped porous boron nitride: metal-free adsorbents for sulfur removal from fuels. J Mater Chem A 2015;3(24):12738–47.
|
| [30] |
Nag A, Raidongia K, Hembram KPSS, Datta R, Waghmare UV, Rao CNR. Graphene analogues of BN: novel synthesis and properties. ACS Nano 2010;4 (3):1539–44.
|
| [31] |
Yan Z, Lin J, Yuan X, Song T, Yu C, Liu Z, et al. Desulfurization of model oil by selective adsorption over porous boron nitride fibers with tailored microstructures. Sci Rep 2017;7(1):3297.
|
| [32] |
Kinaci A, Haskins JB, Sevik C, Cagin T. Thermal conductivity of BN–C nanostructures. Phys Rev B 2012;86(11):115410.
|
| [33] |
D’yachkov EP, D’yachkov PN. Electronic structure of doped boron nitride nanotubes as potential catalysts of photochemical water splitting. Russ J Inorg Chem 2018;63(9):1204–10.
|
| [34] |
Huang C, Chen C, Zhang M, Lin L, Ye X, Lin S, et al. Carbon-doped BN nanosheets for metal-free photoredox catalysis. Nat Commun 2015;6(1):7698.
|
| [35] |
Chen SR, Li P, Xu ST, Pan XL, Fu Q, Bao XH. Carbon doping of hexagonal boron nitride porous materials toward CO2 capture. J Mater Chem A 2018;6 (4):1832–9.
|
| [36] |
Pang J, Chao Y, Chang H, Li H, Xiong J, He M, et al. Tuning electronic properties of boron nitride nanoplate via doping carbon for enhanced adsorptive performance. J Colloid Interface Sci 2017;508:121–8.
|
| [37] |
Lu Q, Zhao Q, Yang TY, Zhai CB, Wang DX, Zhang MZ. Preparation of boron nitride nanoparticles with oxygen doping and a study of their roomtemperature ferromagnetism. ACS Appl Mater Interfaces 2018;10 (15):12947–53.
|
| [38] |
Lei W, Zhang H, Wu Y, Zhang B, Liu D, Qin S, et al. Oxygen-doped boron nitride nanosheets with excellent performance in hydrogen storage. Nano Energy 2014;6:219–24.
|
| [39] |
Weng Q, Kvashnin DG, Wang X, Cretu O, Yang Y, Zhou M, et al. Tuning of the optical, electronic, and magnetic properties of boron nitride nanosheets with oxygen doping and functionalization. Adv Mater 2017;29(28):1700695.
|
| [40] |
Liu F, Li S, Yu DF, Su YP, Shao NN, Zhang ZT. Template-free synthesis of oxygendoped bundlelike porous boron nitride for highly efficient removal of heavy metals from wastewater. ACS Sustain Chem Eng 2018;6(12):16011–20.
|
| [41] |
Xiong J, Yang L, Chao Y, Pang J, Zhang M, Zhu W, et al. Boron nitride mesoporous nanowires with doped oxygen atoms for the remarkable adsorption desulfurization performance from fuels. ACS Sustain Chem Eng 2016;4(8):4457–64.
|
| [42] |
Qu Z, Wu Y, Zhu S, Yu Y, Huo M, Zhang L, et al. Green synthesis of magnetic adsorbent using groundwater treatment sludge for tetracycline adsorption. Engineering 2019;5(5):880–7.
|
| [43] |
Bagali SS, Gowrishankar BS, Roy AS. Optimization, kinetics, and equilibrium studies on the removal of lead (II) from an aqueous solution using banana pseudostem as an adsorbent. Engineering 2017;3(3):409–15.
|
| [44] |
Song Q, Liang J, Fang Yi, Cao C, Liu Z, Li L, et al. Selective adsorption behavior/ mechanism of antibiotic contaminants on novel boron nitride bundles. J Hazard Mater 2019;364:654–62.
|
| [45] |
Li Y, Tian X, Yang W, Li Q, Hou L, Zhu Z, et al. Dielectric composite reinforced by in-situ growth of carbon nanotubes on boron nitride nanosheets with high thermal conductivity and mechanical strength. Chem Eng J 2019;358:718–24.
|
| [46] |
Luo J, Xiong J, Chao Y, Li X, Li H, Pang J, et al. Activated boron nitride ultrathin nanosheets for enhanced adsorption desulfurization performance. J Taiwan Inst Chem Eng 2018;93:245–52.
|
| [47] |
Gautam C, Tiwary CS, Jose S, Brunetto G, Ozden S, Vinod S, et al. Synthesis of low-density, carbon-doped, porous hexagonal boron nitride solids. ACS Nano 2015;9(12):12088–95.
|
| [48] |
Luo J, Chao Y, Tang Z, Hua M, Li X, Wei Y, et al. Design of Lewis acid centers in bundlelike boron nitride for boosting adsorptive desulfurization performance. Ind Eng Chem Res 2019;58(29):13303–12.
|
| [49] |
Shi YW, Zhang XW, Liu GZ. Activated carbons derived from hydrothermally carbonized sucrose: remarkable adsorbents for adsorptive desulfurization. ACS Sustain Chem Eng 2015;3(9):2237–46.
|
| [50] |
Seredych M, Lison J, Jans U, Bandosz TJ. Textural and chemical factors affecting adsorption capacity of activated carbon in highly efficient desulfurization of diesel fuel. Carbon 2009;47(10):2491–500.
|
| [51] |
Chen X, Zhang M, Wei Y, Li H, Liu J, Zhang Q, et al. Ionic liquid-supported 3DOM silica for efficient heterogeneous oxidative desulfurization. Inorg Chem Front 2018;5(10):2478–85.
|
| [52] |
Moon OM, Kang BC, Lee SB, Boo JH. Temperature effect on structural properties of boron oxide thin films deposited by MOCVD method. Thin Solid Films 2004;464:164–9.
|
| [53] |
Weng Q, Ide Y, Wang X, Wang X, Zhang C, Jiang X, et al. Design of BN porous sheets with richly exposed (002) plane edges and their application as TiO2 visible light sensitizer. Nano Energy 2015;16:19–27.
|
| [54] |
Li H, Zhu S, Zhang M, Wu P, Pang J, Zhu W, et al. Tuning the chemical hardness of boron nitride nanosheets by doping carbon for enhanced adsorption capacity. ACS Omega 2017;2(9):5385–94.
|
| [55] |
Xiong J, Yang L, Chao Y, Pang J, Wu P, Zhang M, et al. A large number of low coordinated atoms in boron nitride for outstanding adsorptive desulfurization performance. Green Chem 2016;18(10):3040–7.
|
| [56] |
Tan P, Xue DM, Zhu J, Jiang Y, He QX, Hou ZF, et al. Hierarchical N-doped carbons from designed N-rich polymer: adsorbents with a record-high capacity for desulfurization. AIChE J 2018;64(11):3786–93.
|
| [57] |
Lee D, Lee B, Park KH, Ryu HJ, Jeon S, Hong SH. Scalable exfoliation process for highly soluble boron nitride nanoplatelets by hydroxide-assisted ball milling. Nano Lett 2015;15(2):1238–44.
|
| [58] |
Lv C, Qian Y, Yan C, Ding Y, Liu Y, Chen G, et al. Defect engineering metal-free polymeric carbon nitride electrocatalyst for effective nitrogen fixation under ambient conditions. Angew Chem Int Ed 2018;57(32): 10246–50.
|
| [59] |
Yang SJ, Cho JH, Oh GH, Nahm KS, Park CR. Easy synthesis of highly nitrogenenriched graphitic carbon with a high hydrogen storage capacity at room temperature. Carbon 2009;47(6):1585–91.
|
| [60] |
Weng Q, Wang B, Wang X, Hanagata N, Li X, Liu D, et al. Highly water-soluble, porous, and biocompatible boron nitrides for anticancer drug delivery. ACS Nano 2014;8(6):6123–30.
|
| [61] |
Liu FJ, Huang K, Wu Q, Dai S. Solvent-free self-assembly to the synthesis of nitrogen-doped ordered mesoporous polymers for highly selective capture and conversion of CO2. Adv Mater 2017;29(27): 1700445.
|
| [62] |
Chang H, Chao Y, Pang J, Li H, Lu L, He M, et al. Advanced overlap adsorption model of few-layer boron nitride for aromatic organic pollutants. Ind Eng Chem Res 2018;57(11):4045–51.
|
| [63] |
Xiong J, Zhu W, Li H, Ding W, Chao Y, Wu P, et al. Few-layered graphene-like boron nitride induced a remarkable adsorption capacity for dibenzothiophene in fuels. Green Chem 2015;17(3):1647–56.
|
/
| 〈 |
|
〉 |
