钕改性铁基催化剂用于氮氧化物脱除

doi:10.19964/j.issn.1006-4990.2022-0366

Abstract

Abstract:

Metal Fe and Nd were introduced into the surface of commercial TiO₂ by stepwise impregnation to study its denitrification performance.The samples were characterized by X-ray diffraction（XRD），nitrogen adsorption-desorption（N₂-BET），X-ray photoelectron spectroscopy（XPS），ammonia temperature-programmed desorption（NH₃-TPD），hydrogen temperature-programmed reduction（H₂-TPR）.The adsorption and desorption of N₂ showed that the introduction of Nd reduced the specific surface area of the catalysts loaded with Fe.X-ray diffraction analysis showed that the introduced metal species had good dispersion on the catalyst surface.The results of NH₃-TPD test showed that the introduction of Nd increased the total acid content of the catalyst and changed the acid distribution of the catalyst.XPS results showed that Nd modification increased the content of oxygen and Fe²⁺ on the surface of the catalyst，which was beneficial to the denitrification reaction.H₂-TPR test showed that the introduction of Nd reduced the redox performance of the catalyst slightly.The results of activity test showed that appropriate Nd loading was beneficial to improve the denitrification performance of the catalyst.When the mass fraction of Nd element in the catalyst was 9%，the catalyst had the best denitrification efficiency of 81.4%.

Key words: selective catalytic reduction, supported catalyst, neodymium, Fe-based catalyst

CLC Number:

O643.3

LI Peng, YANG Siyuan, LUO Shizhong, DU Peining, TAN Renjun, JING Fangli. Neodymium-modified iron-based catalysts for nitrogen oxides removal[J]. Inorganic Chemicals Industry, 2023, 55(3): 140-146.

Figures/Tables 13

Fig.1

Table 1

Fig.2

Table 2

Fig.3

Table 3

Fig.4

Fig.5

Table 4

Fig.6

Fig.7

Table 5

Fig.8

References 13

1	ZHANG Runduo， LIU Ning， LEI Zhigang，et al.Selective transformation of various nitrogen-containing exhaust gases toward N₂ over zeolite catalysts[J].Chemical Reviews，2016，116（6）:3658-3721.
2	BAE S W， ROH S A， KIM S D.NO removal by reducing agents and additives in the selective non-catalytic reduction（SNCR） process[J].Chemosphere，2006，65（1）:170-175.
3	FANG De， QI Kai， LI Fengxiang.Excellent sulfur tolerance performance over Fe-SO₄/TiO₂ catalysts for NH₃-SCR:Influence of sulfation and Fe-based sulfates[J].Journal of Environmental Chemical Engineering，2022，10（1）.Doi:10.1016/j.jece.2021.107038.
4	WANG Fang， GUI Keting， YAO Guihuan.The comparison of selective catalytic reduction of de-NO _x on iron-based materials[C]//Asia-Pacific Power and Energy Engineering Conference （APPEEC），2009:2434-2436.
5	KATO A， MATSUDA S， KAMO T，et al.Reaction between NO _x and NH₃ on iron oxide-titanium oxide catalyst[J].The Journal of Physical Chemistry，1981，85（26）:4099-4102.
6	HUANG Li， ZONG Yuhao， WANG Hu，et al.Effect of neodymium addition on plate-type V₂O₅-MoO₃/TiO₂ catalyst for selective catalytic reduction of NO[J].Rare Metal Materials and Engineering，2021，50（2）:0475-0482.
7	XIE Shangzhi， LI Lulu， JIN Lijian，et al.Low temperature high activity of M（M=Ce，Fe，Co，Ni） doped M-Mn/TiO₂ catalysts for NH₃-SCR and in situ DRIFTS for investigating the reaction mechanism[J].Applied Surface Science，2020，515.Doi:10.1016/j.apsusc.2020.146014.
8	WU Xu， WANG Ruonan， DU Yaili，et al.Performance enhancement of NH₃-SCR via employing hydrotalcite-like precursor to induce the decoration of NiO by TiO₂ phase[J].Molecular Catalysis，2019，467:150-160.
9	THIRUPATHI B， SMIRNIOTIS P G.Nickel-doped Mn/TiO₂ as an efficient catalyst for the low-temperature SCR of NO with NH₃:Catalytic evaluation and characterizations[J].Journal of Catalysis，2012，288:74-83.
10	FAN Zhaoyang， SHI Jianwen， GAO Chen，et al.Gd-modified MnO_x for the selective catalytic reduction of NO by NH₃:The promoting effect of Gd on the catalytic performance and sulfur resistance[J].Chemical Engineering Journal，2018，348:820-830.
11	MA Ziran， WU Xiaodong， FENG Ya，et al.Effects of WO₃ doping on stability and N₂O escape of MnO _x -CeO₂ mixed oxides as a low-temperature SCR catalyst[J].Catalysis Communications，2015，69:188-192.
12	XIE Shangzhi， LI Lulu， JIN Lijian，et al.Low temperature high activity of M（M=Ce，Fe，Co，Ni） doped M-Mn/TiO₂ catalysts for NH₃-SCR and in situ DRIFTS for investigating the reaction mechanism[J].Applied Surface Science，2020，515.Doi:10.1016/j.apsusc.2020.146014.
13	WU Jiahui， JIN Shuanglin， WEI Xudong，et al.Enhanced sulfur resistance of H₃PW₁₂O₄₀-modified Fe₂O₃ catalyst for NH₃-SCR:Synergistic effect of surface acidity and oxidation ability[J].Che-mical Engineering Journal，2021，412.Doi:10.1016/j.cej.2021.128712.

催化剂	D_A/nm	D_B/nm
TiO₂	50.1	51.8
Fe-TiO₂	58.3	59.1
1.8%Nd-Fe/TiO₂	58.9	47.4
9%Nd-Fe/TiO₂	61.2	52.3
18%Nd-Fe/TiO₂	55.8	54.5

催化剂	S_BET/（m²·g^-1）	V_P/（cm³·g^-1）	D_BJH/nm
TiO₂	12.2	0.05	15.9
Fe-TiO₂	22.5	0.11	18.7
1.8%Nd-Fe/TiO₂	20.8	0.10	19.7
9%Nd-Fe/TiO₂	15.6	0.08	20.4
18%Nd-Fe/TiO₂	14.3	0.07	19.3

催化剂	NH₃脱附量/（mmol·g^-1）
催化剂	150~300 ℃	300~600 ℃	600~800 ℃	总计
TiO₂	0.006	0.003	—	0.009
Fe-TiO₂	—	0.009	—	0.009
1.8%Nd-Fe/TiO₂	—	0.025	—	0.025
9%Nd-Fe/TiO₂	0.010	0.019	0.006	0.035
18%Nd-Fe/TiO₂	0.009	0.045	0.016	0.070

催化剂	n（Fe²⁺）/n（Fe³⁺）	n（O_Ⅰ）/n（O_Ⅱ）/n（O_Ⅲ）
Fe-TiO₂	69.5/30.5	19.2/77.3/3.5
1.8%Nd-Fe/ TiO₂	76.0/24.0	19.3/73.2/7.5
9%Nd-Fe/ TiO₂	79.9/20.1	27.6/63.1/9.3
18%Nd-Fe/ TiO₂	79.5/20.5	25.6/48.8/25.6

催化剂	H₂消耗量/（mmol·g^-1）
催化剂	100~550 ℃	550~800 ℃	总计
Fe-TiO₂	2.42	—	2.42
1.8%Nd-Fe/ TiO₂	1.49	1.68	3.17
9%Nd-Fe/ TiO₂	0.50	2.54	3.04
18%Nd-Fe/ TiO₂	1.52	1.49	3.01

National Inorganic Salts Information Center

Inorganic Acid-Base-Salt Committee of CIESC

Neodymium-modified iron-based catalysts for nitrogen oxides removal

RichHTML

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 13

References 13

Related Articles 10

Metrics

Comments

Recommended 0

[1]	GUAN Zhiyuan,ZHANG Xiaowei,WANG Mitang,ZHANG Dongliang,ZHU Changle. Effect of rare earth element of Ce and Nd co-doped with zinc oxide on photocatalytic performance of degradation of Rhodamine B [J]. Inorganic Chemicals Industry, 2022, 54(10): 155-162.
[2]	Huang Li,Wang Hu,Zong Yuhao,Chang Zhengfeng,Liu Yang,Li Jinke,Han Pei. Study on deactivation effect of chromium on industrial V-Mo/Ti De-NO_x catalyst [J]. Inorganic Chemicals Industry, 2021, 53(8): 112-116.
[3]	Ye Xieweiyi,Zheng Zhiping,Kuang Qin. Preparation of 2D leaf-like Fe-NC materials derived from ZIF-L and study on their oxygen reduction catalytic performance [J]. Inorganic Chemicals Industry, 2021, 53(6): 1-7.
[4]	HAN Xinyu,LIU Kaijie,BIAN Mengyao,ZHANG Yibo,YANG Xiangguang. Catalytic performance study of Ce-MnO_x for low-temperature purification of nitrogen oxides and carbon monoxide [J]. Inorganic Chemicals Industry, 2021, 53(12): 35-42.
[5]	SONG Jin,WU Fenglong,WANG Yuejun. Study on preparation of Fe/modified MCM-41 catalyst with different loading methods and degradation of methylene blue [J]. Inorganic Chemicals Industry, 2021, 53(11): 122-128.
[6]	Gong Peng,Zhang Bing,Liu Sihao. Status of regeneration and resource utilization of deactivated commercial SCR catalyst [J]. Inorganic Chemicals Industry, 2021, 53(1): 14-17.
[7]	LU Bo, YAO Wen-Li, DENG Pan, LI Ping. Synthesis of nano-sized neodymium oxide by precipitation method with ammonium oxalate [J]. INORGANICCHEMICALSINDUSTRY, 2016, 48(7): 36-.
[8]	YU Xiao-Fei, BAO Xin-Xia, LI Qi-Ming, LI Fang, CHEN Ping. Preparation of Al2O3 supported CoB amorphous alloy catalyst and its application in hydrogen generation [J]. INORGANICCHEMICALSINDUSTRY, 2015, 47(1): 59-.
[9]	WU Qi-Sheng- , CHEN Yi-Lin- . Synthesis， characterization，and de-NOx performance of lanthanum-doped MCM-41 [J]. INORGANICCHEMICALSINDUSTRY, 2014, 46(7): 71-.
[10]	Liao Jing;Han Chen;Ren Shuang;Wang Xiaojuan;Zong Jun. Synthesis and performances of nano-sized neodymium oxide [J]. INORGANICCHEMICALSINDUSTRY, 2009, 0(1): 0-0.