Synergistic biochar photocatalytic oxidation-adsorption for nitrite degradation

doi:10.16085/j.issn.1000-6613.2023-1190

Abstract

Abstract:

The pattern of nitrite removal in different environments under the combined effect of biochar-light-oxygen was studied by orthogonal tests. Combining with multiple contrast tests, the differences in the effects of light, aeration and biochar addition on nitrite removal were analyzed, and the nitroso-nitrogen migration pathways and degradation mechanisms were revealed. The results showed that removal efficiencies of nitrite were mainly influenced by environmental pH and temperature. The pH was the main controlling factor. The highest removal rate was 98.25% at 1.8mg/L nitrite concentration, 0.4g biochar addition, 25℃, 60min reaction time, and pH=2. Aeration normally facilitated the removal of nitrite. The removal rate could be increased at a maximum of 9.7 times compared to non-aerated treatment. Likewise, light promoted the removal of nitrite in strong acidic and alkaline environments, increasing the removal rate at most 5.7 times without light conditions. The addition of biochar brought a weak boost to nitrite removal and needs to be combined with light and aeration to achieve a better removal effect. The coexistence of the three conditions produced a synergistic effect of biochar photocatalytic oxidation-adsorption, which promoted the degradation and migration of nitrite nitrogen through oxidation, photocatalysis and adsorption to obtain a good removal effect.

Key words: photocatalysis, oxidation, adsorption, biochar, nitrite, aeration

摘要：

通过正交实验研究生物炭-光-氧共同作用下不同环境亚硝酸盐净化规律，结合多重对照实验，解析光照、曝气、添加生物炭对亚硝酸盐降解的影响差异，揭示亚硝态氮迁移路径与降解机制。结果表明，亚硝酸盐净化效果主要受环境酸碱度和温度影响，其中酸碱度为主控因素。当亚硝酸盐浓度1.8mg/L、生物炭添加量0.4g、温度25℃、反应时间60min、pH=2时，净化率最高可达98.25%。多数情况下，曝气能够显著提升亚硝酸盐净化率，较之未曝气处理最高提升9.7倍。光照则更适合用于强酸、强碱环境中亚硝酸盐的去除，较之无光照条件净化率最高提升5.7倍。而单纯添加生物炭对亚硝酸盐降解助力效果有限，需配合光照和曝气共同作用。三种条件共存，产生生物炭光催化氧化-吸附协同作用，促使亚硝态氮经由氧化、光催化、吸附等路径降解、迁移，获得良好净化效果。

关键词: 光催化, 氧化, 吸附, 生物炭, 亚硝酸盐, 曝气

CLC Number:

S214

MAO Huakai, YU Yang, ZHANG Yue, XIA Guangkun, WU Yuntao, LOU Leyao, NIU Wenjuan, LIU Nian. Synergistic biochar photocatalytic oxidation-adsorption for nitrite degradation[J]. Chemical Industry and Engineering Progress, 2024, 43(8): 4757-4765.

毛华恺, 余洋, 张悦, 夏广坤, 吴赟韬, 楼乐瑶, 牛文娟, 刘念. 生物炭光催化氧化-吸附协同降解亚硝酸盐[J]. 化工进展, 2024, 43(8): 4757-4765.

Figures/Tables 12

References 39

1	BASAK Bikram, BHUNIA Biswanath, DUTTA Subhasish, et al. Enhanced biodegradation of 4-chlorophenol by Candida tropicalis PHB5 via optimization of physicochemical parameters using Taguchi orthogonal array approach[J]. International Biodeterioration & Biodegradation, 2013, 78: 17-23.
2	AMORIM Camila C, LEÃO Mônica M D, MOREIRA Regina F P M, et al. Performance of blast furnace waste for azo dye degradation through photo-Fenton-like processes[J]. Chemical Engineering Journal, 2013, 224(1): 59-66.
3	于兵川, 吴洪特, 张万忠. 光催化纳米材料在环境保护中的应用[J]. 石油化工, 2005, 34(5): 491-495.
	YU Bingchuan, WU Hongte, ZHANG Wanzhong. Application of nano-photocatalysts in environmental protection[J]. Petrochemical Technology, 2005, 34(5): 491-495.
4	WANG Hao, WANG Jing, XIANG Xin, et al. Preparation of PVDF/CdS/Bi₂WO₆/ZnO hybrid membrane with enhanced visible-light photocatalytic activity for degrading nitrite in water[J]. Environmental Research, 2020, 191: 110036.
5	BOUKHEMIKHEM Z, REKHILA G, BRAHIMI R, et al. Photocatalytic NO₂-oxidation on the hetero-junction Ag(5%)/NiFe₂O₄ prepared by sol gel route[J]. Journal of Photochemistry and Photobiology A: Chemistry, 2020, 394: 112454.
6	FU Dongying, HAN Gaoyi, CHANG Yunzhen, et al. The synthesis and properties of ZnO-graphene nano hybrid for photodegradation of organic pollutant in water[J]. Materials Chemistry and Physics, 2012, 132(2/3): 673-681.
7	魏宏斌, 徐迪民. 固定相TiO₂膜的制备及其光催化活性[J]. 中国给水排水, 2002, 18(7): 57-59.
	WEI Hongbin, XU Dimin. Preparation and photocatalytic activity of fixed phase TiO₂ film[J]. China Water & Wastewater, 2002,18(7): 57-59.
8	ZHANG Lei, JIANG Daochuan, IRFAN Rana Muhammad, et al. Highly efficient and selective photocatalytic dehydrogenation of benzyl alcohol for simultaneous hydrogen and benzaldehyde production over Ni-decorated Zn_0.5Cd_0.5S solid solution[J]. Journal of Energy Chemistry, 2019, 30(3): 71-77.
9	LI Xin, LIN Jing, ZHANG Di, et al. Material flow analysis of titanium dioxide and sustainable policy suggestion in China[J]. Resources Policy, 2020, 67: 101685.
10	SAJAN Chimmikuttanda Ponnappa, WAGEH Swelm, AL-GHAMDI Ahmed A, et al. TiO₂ nanosheets with exposed {001} facets for photocatalytic applications[J]. Nano Research, 2016, 9(1): 3-27.
11	LU Haiqiang, ZHAO Jianghong, LI Li, et al. Selective oxidation of sacrificial ethanol over TiO₂-based photocatalysts during water splitting[J]. Energy & Environmental Science, 2011, 4(9): 3384-3388.
12	YASUDA Masahide, MATSUMOTO Tomoko, YAMASHITA Toshiaki. Sacrificial hydrogen production over TiO₂-based photocatalysts: Polyols, carboxylic acids, and saccharides[J]. Renewable and Sustainable Energy Reviews, 2018, 81: 1627-1635.
13	TESTA Juan J, GRELA María A, LITTER Marta I. Heterogeneous photocatalytic reduction of chromium(Ⅵ) over TiO₂ particles in the presence of oxalate: Involvement of Cr(Ⅴ) species[J]. Environmental Science & Technology, 2004, 38(5): 1589-1594.
14	陈杰, 肖玉婷, 汪楠, 等. 简易合成具有增强电荷转移的Z型CeO₂/C₃N₄异质结用于光催化CO₂还原[J]. Science China Materials, 2023, 66(8): 3165-3175.
	CHEN Jie, XIAO Yuting, WANG Nan, et al. Facile synthesis of a Z-scheme CeO₂/C₃N₄ heterojunction with enhanced charge transfer for CO₂ photoreduction[J]. Science China Materials, 2023, 66(8): 3165-3175.
15	LUO Jinhua, WU Yaohui, JIANG Mengzhu, et al. Novel ZnFe₂O₄/BC/ZnO photocatalyst for high-efficiency degradation of tetracycline under visible light irradiation[J]. Chemosphere, 2023, 311(1): 137041.
16	XIA Qi, HUANG Binbin, YUAN Xingzhong, et al. Modified stannous sulfide nanoparticles with metal-organic framework: Toward efficient and enhanced photocatalytic reduction of chromium (Ⅵ) under visible light[J]. Journal of Colloid and Interface Science, 2018, 530： 481-492.
17	DJELLABI Ridha, YANG Bo, WANG Yan, et al. Carbonaceous biomass-titania composites with TiOC bonding bridge for efficient photocatalytic reduction of Cr(‍Ⅵ) under narrow visible light[J]. Chemical Engineering Journal, 2019, 366: 172-180.
18	Dinh Ngoc Giao NGO, CHUANG Xiangying, HUANG Chin-Pao, et al. Compositional characterization of nine agricultural waste biochars: The relations between alkaline metals and cation exchange capacity with ammonium adsorption capability[J]. Journal of Environmental Chemical Engineering, 2023, 11(3): 110003.
19	HUFF Matthew D, LEE James W. Biochar-surface oxygenation with hydrogen peroxide[J]. Journal of Environmental Management, 2016, 165: 17-21.
20	LIU Yurong, PASKEVICIUS Mark, Veronica SOFIANOS M, et al. A SAXS study of the pore structure evolution in biochar during gasification in H₂O, CO₂ and H₂O/CO₂ [J]. Fuel, 2021, 292: 120384.
21	周石洋, 陈玲. 食品中亚硝酸盐含量测定的研究[J]. 食品安全质量检测学报, 2011, 2(6): 285-289.
	ZHOU Shiyang, CHEN Ling. Study on the determination of nitrite in food[J]. Journal of Food Safety & Quality, 2011, 2(6): 285-289.
22	中华人民共和国自然资源部. 地下水质分析方法硝酸盐的测定紫外分光光度法: [S]. 北京: 中国标准出版社, 2021.
	Ministry of Natural Resources of the People’s Republic of China. Analysis methods for groundwater quality—Determination of nitrate ultraviolet spectrophotometric method: [S]. Beijing: Standards Press of China, 2021.
23	栗秀萍, 于洋, 何旺, 等. 超重力强化AMP-PZ复合溶液脱碳技术及表观动力学[J]. 化工进展, 2022, 41(S1): 22-28.
	LI Xiuping, YU Yang, HE Wang, et al. High-gravity intensified decarburization process and apparent kinetics of AMP-PZ composite solution[J]. Chemical Industry and Engineering Progress, 2022, 41(S1): 22-28.
24	中本一雄, 黄德如. 无机和配位化合物的红外和拉曼光谱[M]. 北京：化学工业出版社,1986.
	KAZUO Nakamoto, HUANG Deru. Inrared and Raman spectra of inorganic and coordination compounds[M]. Beijing: Chemical Industry Press, 1986.
25	黄安香, 杨定云, 杨守禄, 等. 改性生物炭对土壤重金属污染修复研究进展[J]. 化工进展, 2020, 39(12): 5266-5274.
	HUANG Anxiang, YANG Dingyun, YANG Shoulu, et al. Advance in remediation of heavy metal pollution in soil by modified biochar[J]. Chemical Industry and Engineering Progress, 2020, 39(12): 5266-5274.
26	宋江生, 管益东, 师杨杰, 等. 杨木基生物炭吸附去除水溶液中磺胺吡啶[J]. 净水技术, 2023, 42(7): 90-97.
	SONG Jiangsheng, GUAN Yidong, SHI Yangjie, et al. Poplar based biochars for adsorption and removal of sulfapyridine in aqueous solution[J]. Water Purification Technology, 2023, 42(7): 90-97.
27	钟来元, 廖荣骏, 刘付宇杰, 等. KOH改性花生壳生物炭对盐酸四环素的吸附性能及其机理[J]. 农业环境科学学报, 2023, 42(9): 2038-2048.
	ZHONG Laiyuan, LIAO Rongjun, LIUFU Yujie, et al. Adsorption of tetracycline hydrochloride by KOH modified peanut shell biochar and its mechanism[J]. Journal of Agro-Environment Science, 2023, 42(9): 2038-2048.
28	杨婷婷, 黄艳艳, 柳维扬, 等. 三种改性小麦秸秆生物炭表征及其对Cu²⁺的吸附性能[J]. 农业工程学报, 2023, 39(8): 222-230.
	YANG Tingting, HUANG Yanyan, LIU Weiyang, et al. Characterization of three kinds of modified wheat straw derived biochars and their sorption capacity for Cu²⁺ [J]. Transactions of the Chinese Society of Agricultural Engineering, 2023, 39(8): 222-230.
29	王金玉, 王赛男, 卢佳宏, 等. 盐酸改性豆渣不溶性膳食纤维对亚硝酸盐的吸附特性及机理[J]. 大豆科学, 2022, 41(4): 463-471.
	WANG Jinyu, WANG Sainan, LU Jiahong, et al. Adsorption characteristics and mechanism of hydrochloric acid modified okara insoluble dietary fiber to nitrite[J]. Soybean Science, 2022, 41(4): 463-471.
30	庄远红, 刘静娜, 费鹏, 等. 模拟胃环境下柚皮果胶对亚硝酸根的吸附动力学[J]. 西南大学学报(自然科学版), 2018, 40(12): 65-72.
	ZHUANG Yuanhong, LIU Jingna, FEI Peng, et al. Adsorption kinetics of pectin from pomelo peelon nitrite in a simulated gastric environment[J]. Journal of Southwest University(Natural Science Edition), 2018, 40(12): 65-72.
31	吴丹萍, 陈全, 李东梅, 等. 生物炭含氧官能团的生成溯源及其在污染物吸附-降解过程中的作用[J]. 环境化学, 2021, 40(10): 3190-3198.
	WU Danping, CHEN Quan, LI Dongmei, et al. Traceability of oxygen-containing functional groups in biochars and their roles in the adsorption-degradation of contaminants[J]. Environmental Chemistry, 2021, 40(10): 3190-3198.
32	向欣. CdS/Bi₂S₃/Bi₂MoO₆光催化膜耦合芽孢杆菌协同降解亚硝酸盐[D]. 南宁：广西大学, 2021.
	XIANG Xin. Synergistic Degradation of nitrite by CdS/Bi₂S₃/Bi₂MoO₆ photocatalytic membrane coupled bacillus[D]. Nanning: Guangxi University, 2021.
33	GOMAA Hosam M, SAUDI H A, YAHIA I S, et al. Influence of graphene nanopowder impurities on the structural and optical properties of sodium borate copper-based glass: Towards UV/NIR shielding materials[J]. Solid State Sciences, 2022, 129: 106911.
34	李法云, 李佳宇, 吝美霞, 等. 大豆秸秆生物炭负载石墨相氮化碳对土壤石油烃的光催化降解[J]. 应用基础与工程科学学报, 2022, 30(3): 519-529.
	LI Fayun, LI Jiayu, LIN Meixia, et al. Photocatalytic degradation of soil petroleum hydrocarbons by biochar supported graphite phase carbon nitride[J]. Journal of Basic Science and Engineering, 2022, 30(3): 519-529.
35	曹雪娟, 单柏林, 邓梅, 等. Fe掺杂g-C₃N₄光催化剂的制备及光催化性能研究[J]. 重庆交通大学学报(自然科学版), 2019, 38(11): 52-57.
	CAO Xuejuan, SHAN Bailin, DENG Mei, et al. Preparation and photocatalytic properties of Fe-doped g-C₃N₄ photocatalyst[J]. Journal of Chongqing Jiaotong University(Natural Science), 2019, 38(11): 52-57.
36	高晓明, 付峰, 吕磊, 等. 光催化剂Cu-BiVO₄的制备及其光催化降解含酚废水[J]. 化工进展, 2012, 31(5): 1039-1042, 1087.
	GAO Xiaoming, FU Feng, Lei LYU, et al. Preparation of Cu-BiVO₄ photocatalyst and its application in the treatment of phenol-containing wastewater[J]. Chemical Industry and Engineering Progress, 2012, 31(5): 1039-1042, 1087.
37	王宏娟, 郑楠, 董晓丽. 碘掺杂氯氧化铋光催化剂的制备及性能[J]. 大连工业大学学报, 2020, 39(6): 419-423.
	WANG Hongjuan, ZHENG Nan, DONG Xiaoli. Preparation and properties of I-doped bismuth chloride oxide photocatalyst[J]. Journal of Dalian Polytechnic University, 2020, 39(6): 419-423.
38	李红亮, 张涛, 付贤军, 等. ZnO/g-C₃N₄复合光催化材料降解四环素研究[J]. 能源与环保, 2023, 45(8): 163-169.
	LI Hongliang, ZHANG Tao, FU Xianjun, et al. Study on degradation of tetracycline by ZnO/g-C₃N₄ composite photocatalytic materials[J]. China Energy and Environmental Protection, 2023, 45(8): 163-169.
39	赵文武, 周海静, 黄雁, 等. 稀土掺杂硼酸盐Bi₂ZnB₂O₇∶xDy³⁺光催化剂的合成及其催化机理[J]. 化工进展, 2022, 41(11): 5843-5849.
	ZHAO Wenwu, ZHOU Haijing, HUANG Yan, et al. Photocatalytic mechanism and synthesis of rare earth doped borate Bi₂ZnB₂O₇∶xDy³⁺ photocatalyst[J]. Chemical Industry and Engineering Progress, 2022, 41(11): 5843-5849.

元素组成	质量分数/%
C	42.72
H	2.58
O	47.79
N	1.20
S	0.55
K	1.43
Ca	0.57
Mg	0.78

元素组成	质量分数/%
C	42.72
H	2.58
O	47.79
N	1.20
S	0.55
K	1.43
Ca	0.57
Mg	0.78

水平	α/mg·L^-1	β/g	γ/℃	δ	ε/min
1	0.6	0.2	25	2	20
2	1.8	0.4	30	4	60
3	5.4	0.6	35	6	100
4	16.2	0.8	40	8	140
5	48.6	1.0	45	10	180

水平	α/mg·L^-1	β/g	γ/℃	δ	ε/min
1	0.6	0.2	25	2	20
2	1.8	0.4	30	4	60
3	5.4	0.6	35	6	100
4	16.2	0.8	40	8	140
5	48.6	1.0	45	10	180

试验组	编号	L	A	B	pH	酸碱度
LABO	LABO1	√	√	√	3	强酸
LABO	LABO2	√	√	√	6.5	弱酸
LABO	LABO3	√	√	√	7	中性
LABO	LABO4	√	√	√	7.5	弱碱
LABO	LABO5	√	√	√	9	强碱
ABO	ABO1	×	√	√	3	强酸
ABO	ABO2	×	√	√	6.5	弱酸
ABO	ABO3	×	√	√	7	中性
ABO	ABO4	×	√	√	7.5	弱碱
ABO	ABO5	×	√	√	9	强碱
LBO	LBO1	√	×	√	3	强酸
LBO	LBO2	√	×	√	6.5	弱酸
LBO	LBO3	√	×	√	7	中性
LBO	LBO4	√	×	√	7.5	弱碱
LBO	LBO5	√	×	√	9	强碱
LAO	LAO1	√	√	×	3	强酸
LAO	LAO2	√	√	×	6.5	弱酸
LAO	LAO3	√	√	×	7	中性
LAO	LAO4	√	√	×	7.5	弱碱
LAO	LAO5	√	√	×	9	强碱
BO	BO1	×	×	√	3	强酸
BO	BO2	×	×	√	6.5	弱酸
BO	BO3	×	×	√	7	中性
BO	BO4	×	×	√	7.5	弱碱
BO	BO5	×	×	√	9	强碱
AO	AO1	×	√	×	3	强酸
AO	AO2	×	√	×	6.5	弱酸
AO	AO3	×	√	×	7	中性
AO	AO4	×	√	×	7.5	弱碱
AO	AO5	×	√	×	9	强碱
LO	LO1	√	×	×	3	强酸
LO	LO2	√	×	×	6.5	弱酸
LO	LO3	√	×	×	7	中性
LO	LO4	√	×	×	7.5	弱碱
LO	LO5	√	×	×	9	强碱
O	O1	×	×	×	3	强酸
O	O2	×	×	×	6.5	弱酸
O	O3	×	×	×	7	中性
O	O4	×	×	×	7.5	弱碱
O	O5	×	×	×	9	强碱