摘要
为实现蓝藻水华(CBB)的资源化利用,开发2,5-二甲酰呋喃(DFF)的绿色催化合成技术,将CBB高温炭化制成蓝藻基氮杂化活性炭(N-AC-CB),用于催化O_(2)氧化5-羟甲糠醛(HMF)合成DFF反应。采用XRD、Raman、BET、FTIR、XPS对N-AC-CB进行了表征,考察了CBB炭化温度和反应条件(反应温度、时间、氧压、溶剂)对反应的影响。结果表明,炭化温度700℃制备的N-AC-CB-700具有较好的催化性能,其所含石墨型氮杂化结构对形成催化活性中心起重要作用,总氮含量(5.90%)和石墨型氮含量(1.83%)均最高;在以6.37 g(0.05 mol)HMF为原料、1.20 g N-AC-CB-700为催化剂、150 mL N,N-二甲基乙酰胺为溶剂、反应温度100℃、氧压1.25 MPa、反应时间10 h的最优反应条件下,HMF转化率为100.0%,DFF收率为92.8%。N-AC-CB-700循环使用7次后,催化活性与首次使用相比仅下降5.4%,循环使用9次后,催化活性下降13.3%。
To achieve the resource utilization of cyanobacterial blooms(CBB)and develop green catalytic synthesis technology for 2,5-diformyl furan(DFF),N-doped active carbon(N-AC-CB)was prepared from high-temperature carbonization of CBB,characterized by XRD,Raman,BET,FTIR and XPS,and used for catalysis over aerobic oxidation of 5-hydroxymethylfurfural(HMF),with the influence of CBB carbonization temperature and reaction conditions(reaction temperature,time,oxygen pressure,solvent)on the reaction evaluated.The results showed that the N-AC-CB-700 obtained from carbonization of CBB at 700℃displayed good catalytic performance,and the graphite-type nitrogen hybrid structure in it played an important role in the formation of catalytic active centers,with both the total nitrogen content(5.90%)and the graphite type nitrogen content(1.83%)the highest.Under the optimal reaction conditions of 6.37 g(0.05 mol)HMF as raw materials,1.20 g N-AC-CB-700 as catalyst,150 mL N,N-dimethylacetamide as solvent,reaction temperature 100℃,oxygen pressure 1.25 MPa,and reaction time 10 h,the conversion rate of HMF and the yield of DFF reached 100.0%and 92.8%,respectively.The catalytic activity of N-AC-CB-200 only decreased by 5.4%with the catalyst recycled 7 times,while the activity decreased by 13.3%when reused 9 times.
作者
唐凯
司焱光
韩召席
刘平
金刘君
单玉华
TANG Kai;SI Yanguang;HAN Zhaoxi;LIU Ping;JIN Liujun;SHAN Yuhua(School of Petrochemical Engineering,Changzhou University,Changzhou 213164,Jiangsu,China;Advanced Catalysis and Green Manufacturing Collaborative Innovation Center,Changzhou 213164,Jiangsu,China)
出处
《精细化工》
2026年第2期371-378,共8页
Fine Chemicals
基金
江苏省高等教育机构自然科学基金重大项目(23KJA530001)。
关键词
蓝藻水华
氮杂化活性炭
氧气氧化
5-羟甲糠醛
2
5-二甲酰呋喃
催化技术
cyanobacterial blooms
N-doped active carbon
aerobic oxidation
5-hydroxymethylfurfural
2,5-diformylfuran
catalysis technology
