Study on the performance of hydrotalcite-based ozone decomposition catalyst
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摘要: 居室环境内臭氧严重危害人体健康,催化分解法是最有效的臭氧净化技术之一。高活性和稳定性臭氧分解催化剂的开发是关键,特别是在高湿度大空速下,臭氧的低温催化分解具有较高的技术壁垒。层状双金属氢氧化物(LDH)具有独特的二维层状结构,具有灵活的结构可调控性。本实验通过共沉淀法用过渡金属制得Ni3Fe、Ni3Co、Ni3Mn与Co3Fe水滑石结构催化剂,在30 ℃、600000 mL/(g·h)、低湿度RH < 5%和高湿度RH > 90%条件下,测试了其臭氧催化分解性能。结果表明,Ni3Co-LDH在低湿度和高湿度下,都表现出优良的臭氧分解性能,臭氧转化率分别为88%和77%。结合XRD、BET、SEM、XPS、Raman、FT-IR、TG等表征手段,揭示了LDH催化剂优良臭氧分解性能的内在原因机理。本实验的研究为过渡金属臭氧分解催化剂开发提供了新的思路。Abstract: Ozone in the indoor environment is seriously harmful to human health, and the catalytic decomposition method is one of the most effective ozone purification technologies. The development of ozone decomposition catalyst with superior activity and stability is the bottleneck, especially under high humidity, high space velocity, and ambient temperature. Layered double hydroxide (LDH) has a unique two-dimensional layered structure and excellent water resistance. In the paper, Ni3Fe, Ni3Co, Ni3Mn, and Co3Fe hydrotalcite-structured catalysts were prepared by the coprecipitation method. And their ozone catalytic decomposition performance was tested under 30 ℃, 600000 mL/(g·h), low humidity (RH< 5%), and high humidity (RH > 90%). The results showed that Ni3Co-LDH exhibited excellent ozone decomposition performance, and the ozone conversion was 88% and 77% under low humidity and high humidity, respectively. Combined with XRD, BET, SEM, XPS, Raman, FT-IR, TG and other characterizations, the intrinsic mechanism of the excellent ozone decomposition performance of LDH catalysts was revealed. The paper provided new ideas for developing transition metal ozone decomposition catalysts.
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图 7 (a):新鲜及反应后Ni3Co-LDH的Ni 2p XPS谱图;(b):新鲜及反应后的Ni3Fe-LDH Ni 2p XPS谱图;(c):不同LDH新鲜催化剂的Ni 2p XPS谱图;(d):Ni3Mn-LDH的Mn 3s XPS谱图
Figure 7 (a): Ni 2p XPS spectra of fresh and used Ni3Co-LDH; (b): Ni 2p XPS spectra of fresh and used Ni3Fe-LDH; (c): Ni 2p XPS spectra of different LDH catalysts; (d): Mn 3s XPS spectrum of Ni3Mn-LDH
表 1 不同LDH催化剂的织构参数
Table 1 Texture properties of different LDH catalysts
Sample Surface area/(m2·g−1) Pore volume/(cm3·g−1) Pore diameter/nm Ni3Co 140.865 0.1840 3.811 Ni3Mn 81.315 0.3377 3.408 Ni3Fe 96.839 0.2277 3.840 Co3Fe 105.603 0.2926 3.813 表 2 Ni3Co-LDH反应前后的Co2 + 与Co3 + 含量
Table 2 Co2 + and Co3 + contents in fresh and spent Ni3Co-LDH samples
Catalyst Co2 + /% Co3 + /% Ni3Co 63.01 36.99 Ni3Co-G 13.52 86.48 Ni3Co-S 52.87 47.13 表 3 不同催化剂的表面氧物种分析
Table 3 Quantitative analysis of surface oxygen species on different catalysts
Catalyst OOH/Ototal
(%)Oads/Ototal
(%)Olat/Ototal
(%)Ni3Fe 28.98 67.61 3.41 Ni3Co 15.41 83.15 1.44 Ni3Mn 36.40 57.70 5.91 Co3Fe 35.14 58.11 6.76 Ni3Fe-G 53.69 43.74 2.57 Ni3Fe-S 33.29 63.00 3.70 Ni3Co-G 35.12 61.49 3.39 Ni3Co-S 11.53 80.96 7.51 -
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