氮自掺杂污泥炭催化过一硫酸盐氧化去除水中苯酚
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摘要
为了克服纳米碳材料催化剂的不足,以市政污泥为原料热解制备污泥炭作为非均相催化剂,并应用于过一硫酸盐(PMS)反应体系氧化去除水中的苯酚。通过表征和降解试验研究了污泥炭的催化效能。结果表明,污泥炭具有较高的PMS催化性能,在污泥炭SC-B投量为0.5 g/L、PMS投量为10.6 mmol/L、p H值为6.5的条件下,40 min内污泥炭/PMS体系对苯酚的去除率达到了97.7%;污泥炭中氮的含量和组分对催化活性具有较大的影响;使用后的污泥炭可通过外加尿素热解的方式再生。
Nano carbons,such as graphene,are common metal-free heterogeneous PMS catalysts;however,there are challenges in production and cost. Sewage sludge was converted into metal-free heterogeneous PMS catalyst for efficient degradation of phenol in water. The sludge carbons were characterized and assessed through catalytic experiments. Results demonstrated that the prepared SC-B had excellent catalytic effect. When the dosage of SC-B and PMS was 0. 5 g/L and 10. 6 mmol/L,respectively,and the p H was 6. 5,phenol was removed by 97. 7% in 40 min in the SC-B/PMS system. The content and constituent of nitrogen was critical for the catalytic activity of the sludge carbon. The catalyst could be regenerated in co-pyrolysis with urea.
Nano carbons,such as graphene,are common metal-free heterogeneous PMS catalysts;however,there are challenges in production and cost. Sewage sludge was converted into metal-free heterogeneous PMS catalyst for efficient degradation of phenol in water. The sludge carbons were characterized and assessed through catalytic experiments. Results demonstrated that the prepared SC-B had excellent catalytic effect. When the dosage of SC-B and PMS was 0. 5 g/L and 10. 6 mmol/L,respectively,and the p H was 6. 5,phenol was removed by 97. 7% in 40 min in the SC-B/PMS system. The content and constituent of nitrogen was critical for the catalytic activity of the sludge carbon. The catalyst could be regenerated in co-pyrolysis with urea.
引文
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[3]Wang Y,Ao Z,Sun H,et al.Activation of peroxymonosulfate by carbonaceous oxygen groups:experimental and density functional theory calculations[J].Appl Catal B:Environ,2016,198:295-302.
[4]Oh W,Dong Z,Lim T.Generation of sulfate radical through heterogeneous catalysis for organic contaminants removal:Current development,challenges and prospects[J].Appl Catal B:Environ,2016,194:169-201.
[5]Sun H,Liu S,Zhou G,et al.Reduced graphene oxide for catalytic oxidation of aqueous organic pollutants[J].ACS Appl Mater Interfaces,2012,4(10):5466-5471.
[6]Sun H,Kwan C,Suvorova A,et al.Catalytic oxidation of organic pollutants on pristine and surface nitrogen-modified carbon nanotubes with sulfate radicals[J].Appl Catal B:Environ,2014,154/155:134-141.
[7]Liu H,Sun P,Feng M,et al.Nitrogen and sulfur codoped CNT-COOH as an efficient metal-free catalyst for the degradation of UV filter BP-4 based on sulfate radicals[J].Appl Catal B:Environ,2016,187:1-10.
[8]Indrawirawan S,Sun H,Duan X,et al.Low temperature combustion synthesis of nitrogen-doped graphene for metal-free catalytic oxidation[J].J Mater Chem A,2015,3(7):3432-3440.
[9]Duan X,Indrawirawan S,Sun H,et al.Effects of nitrogen-,boron-,and phosphorus-doping or codoping on metal-free graphene catalysis[J].Catalysis Today,2015,249:184-191.
[10]Duan X,Ao Z,Sun H,et al.Nitrogen-doped graphene for generation and evolution of reactive radicals by metalfree catalysis[J].ACS Appl Mater Interfaces,2015,7(7):4169-4178.
[11]Deng D,Pan X,Yu L,et al.Toward N-doped graphene via solvothermal synthesis[J].Chem Mater,2011,23:1188-1193.
[12]Tu Y,Xiong Y,Tian S,et al.Catalytic wet air oxidation of 2-chlorophenol over sewage sludge-derived carbonbased catalysts[J].J Hazard Mater,2014,276:88-96.
[13]Wen G,Pan Z H,Ma J,et al.Reuse of sewage sludge as a catalyst in ozonation-Efficiency for the removal of oxalic acid and the control of bromate formation[J].J Hazard Mater,2012,239/240:381-388.
[14]Tu Y,Tian S,Kong L,et al.Co-catalytic effect of sewage sludge-derived char as the support of Fenton-like catalyst[J].Chem Eng J,2012,185:44-51.
[15]Zhou K,Zhou W,Liu X,et al.Nitrogen self-doped porous carbon from surplus sludge as metal-free electrocatalysts for oxygen reduction reactions[J].ACS Appl Mater Interfaces,2014,6(17):14911-14918.
[16]Gao Y,Hu G,Zhong J,et al.Nitrogen-doped sp2-hybridized carbon as a superior catalyst for selective oxidation[J].Angew Chem Int Ed Eng,2013,52(7):2109-2113.
[17]Tian Y,Zhang J,Zuo W,et al.Nitrogen conversion in relation to NH3and HCN during microwave pyrolysis of sewage sludge[J].Environ Sci Technol,2013,47(7):3498-3505.
[18]Yang S,Li L,Xiao T,et al.Promoting effect of ammonia modification on activated carbon catalyzed peroxymonosulfate oxidation[J].Sep Purif Technol,2016,160:81-88.
[19]Wang C,Kang J,Sun H,et al.One-pot synthesis of Ndoped graphene for metal-free advanced oxidation processes[J].Carbon,2016,102:279-287.
[20]Liu J,Zhao Z,Shao P,et al.Activation of peroxymonosulfate with magnetic Fe3O4-Mn O2core-shell nanocomposites for 4-chlorophenol degradation[J].Chem Eng J,2015,262:854-861.
[21]Yang S,Li L,Xiao T,et al.Reuse performance of granular-activated carbon and activated carbon fiber in catalyzed peroxymonosulfate oxidation[J].Environ Technol Lett,2017,38(5):598-605.
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