Research on modified cyanobacterial biochar promoting cathodic hydrogen autotrophic denitrification in bioelectrochemical system
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摘要:
以太湖蓝藻为原料制备不同种类的活性生物炭,并将其投入到生物电化学系统(BES)的阴极促进氢自养反硝化。通过扫描电镜、能谱仪和傅里叶红外光谱对未经改性(ABC-800)、硝酸改性(ABC-800N)和KOH改性(ABC-800K)3组蓝藻生物炭进行观察,并与不加入蓝藻生物炭的对照组进行比较,以考察生物炭促进BES生物阴极的反硝化过程中的电子传递机制。结果表明:ABC-800N表面的N、O元素含量最高,同时与电子传递能力及生物相容性相关的共轭醌、酮结构的丰度也最高;将蓝藻生物炭投加至BES的非生物阴极中可提高阴极的脱氮效率,ABC-800N投加量为0.5 g时,7 d内脱氮效率达到最高,为96.0%,而对照组仅为29.6%;高通量测序表明,ABC-800N组的优势菌属为Thauera、JGI_0001001_H03、Thiobacillus、Denitratisoma等。
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关键词:
- 生物电化学系统(BES) /
- 氢自养反硝化 /
- 蓝藻生物炭 /
- 高通量测序
Abstract:Different kinds of active biochar were prepared from cyanobacteria in Taihu Lake and put into the cathode of bioelectrochemical system (BES) to promote hydrogen autotrophic denitrification. Three groups of cyanobacterial biochar of Unmodified (ABC-800), modified by nitric acid (ABC-800N) and modified by KOH (ABC-800K) were observed by scanning electron microscopy (SEM), energy dispersive spectrometer (EDS) and Fourier transform infrared spectroscopy (FTIR), and were compared with the control group without the addition of cyanobacteria biochar, to investigate the electron transfer mechanism in denitrification process of biochar promotes BES biocathode. The results showed that the contents of nitrogen and oxygen on ABC-800N surface were the highest, and the abundance of conjugated quinone and ketone structures related to electron transport capacity and biocompatibility was also the highest. Adding cyanobacteria biochar to the abiotic cathode of BES could improve the nitrogen removal efficiency of the cathode. After adding 0.5 g ABC-800N into the BES abiotic cathode, the nitrogen removal efficiency reached the highest within 7 days, which was 96.0%, while the control group was only 29.6%. High-throughput sequencing showed that the dominant bacteria in ABC-800N group were Thauera, JGI_0001001_H03, Thiobacillus, and Denitratisoma, etc.
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表 1 3种生物炭材料表面元素含量
Table 1. Surface element contents of the three biochar materials
% 生物炭 C N O K ABC-800 86.88 6.88 6.24 ABC-800N 67.61 13.27 19.12 ABC-800K 76.78 7.04 15.98 0.2 表 2 投加不同生物炭材料后各组反应器微生物的共有OTU在门水平的相对丰度
Table 2. Relative abundance of shared OTU of microorganisms in each reactor at phylum level after different biochar materials addition
% 细菌门 对照组 ABC-800 ABC-800N ABC-800K Proteobacteria 52.15 37.63 30.96 36.02 Firmicutes 2.63 4.37 4.26 5.38 Chloroflexi 8.32 9.00 11.51 8.62 Bacteroidota 12.91 27.49 28.88 21.89 Actinobacteriota 3.52 9.78 9.33 7.68 Synergisteota 4.20 0.30 0.99 0.56 Acidobacteriota 0.55 2.89 9.08 4.94 -
[1] 杨延梅, 张田, 郑明霞, 等.基于水化学及当地稳定同位素的地下水硝酸盐污染空间分布特征及污染源解析[J]. 环境科学研究,2021,34(9):2164-2172. doi: 10.13198/j.issn.1001-6929.2021.05.21YANG Y M, ZHANG T, ZHENG M X, et al. Spatial distribution characteristics and pollution source analysis of nitrate pollution in groundwater based on hydrochemistry and local stable isotopes[J]. Research of Environmental Sciences,2021,34(9):2164-2172. doi: 10.13198/j.issn.1001-6929.2021.05.21 [2] LOGAN B E, RABAEY K. Conversion of wastes into bioelectricity and chemicals by using microbial electrochemical technologies[J]. Science,2012,337(6095):686-690. doi: 10.1126/science.1217412 [3] LIANG D D, HE W H, LI C, et al. Remediation of nitrate contamination by membrane hydrogenotrophic denitrifying biofilm integrated in microbial electrolysis cell[J]. Water Research,2021,188:116498. doi: 10.1016/j.watres.2020.116498 [4] PARK H I, CHOI Y J, PAK D. Autohydrogenotrophic denitrifying microbial community in a glass beads biofilm reactor[J]. Biotechnology Letters,2005,27(13):949-953. doi: 10.1007/s10529-005-7654-x [5] 许子聪, 李海松, 胡培基.污泥膨胀对反硝化中试反应器效能及菌群结构的影响[J]. 环境工程技术学报,2019,9(2):139-144. doi: 10.12153/j.issn.1674-991X.2018.10.300XU Z C, LI H S, HU P J. The effects of filamentous sludge bulking on performance and bacterial community structure of pilot-scale denitrification reactor[J]. Journal of Environmental Engineering Technology,2019,9(2):139-144. doi: 10.12153/j.issn.1674-991X.2018.10.300 [6] 马金莲, 马晨, 汤佳, 等.电子穿梭体介导的微生物胞外电子传递: 机制及应用[J]. 化学进展,2015,27(12):1833-1840. doi: 10.7536/PC150533MA J L, MA C, TANG J, et al. Mechanisms and applications of electron shuttle-mediated extracellular electron transfer[J]. Progress in Chemistry,2015,27(12):1833-1840. doi: 10.7536/PC150533 [7] 曹璟, 王鹏飞, 陈俊伊, 等.改性生物炭材料原位修复污染底泥的效果[J]. 环境工程技术学报,2020,10(4):661-670. doi: 10.12153/j.issn.1674-991X.20200021CAO J, WANG P F, CHEN J Y, et al. Study on the effect of modified biochar materials on in situ remediation of contaminated sediments[J]. Journal of Environmental Engineering Technology,2020,10(4):661-670. doi: 10.12153/j.issn.1674-991X.20200021 [8] PRADO A, BERENGUER R, ESTEVE A. Electroactive biochar outperforms highly conductive carbon materials for biodegrading pollutants by enhancing microbial extracellular electron transfer[J]. Carbon,2019,146:597-609. doi: 10.1016/j.carbon.2019.02.038 [9] WANG J L, WANG S Z. Preparation, modification and environmental application of biochar: a review[J]. Journal of Cleaner Production,2019,227:1002-1022. doi: 10.1016/j.jclepro.2019.04.282 [10] SU X X, WANG Y Y, HE Q, et al. Biochar remediates denitrification process and N2O emission in pesticide chlorothalonil-polluted soil: role of electron transport chain[J]. Chemical Engineering Journal,2019,370:587-594. doi: 10.1016/j.cej.2019.03.195 [11] 杨秋钰. 阴极强化对BES氢自养反硝化脱氮过程的影响研究[D]. 无锡: 江南大学, 2020. [12] 国家环境保护总局. 水和废水监测分析方法[M]. 4版. 北京: 中国环境科学出版社, 2002. [13] WANG J C, KASKEL S. KOH activation of carbon-based materials for energy storage[J]. Journal of Materials Chemistry,2012,22(45):23710-23725. doi: 10.1039/C2JM34066F [14] DONG X L, MA L Q, ZHU Y J, et al. Mechanistic investigation of mercury sorption by Brazilian pepper biochars of different pyrolytic temperatures based on X-ray photoelectron spectroscopy and flow calorimetry[J]. Environmental Science & Technology,2013,47(21):12156-12164. [15] ZHAO B, O'CONNOR D, ZHANG J L, et al. Effect of pyrolysis temperature, heating rate, and residence time on rapeseed stem derived biochar[J]. Journal of Cleaner Production,2018,174:977-987. doi: 10.1016/j.jclepro.2017.11.013 [16] YANG F, ZHANG S S, LI H P, et al. Corn straw-derived biochar impregnated with α-FeOOH nanorods for highly effective copper removal[J]. Chemical Engineering Journal,2018,348:191-201. doi: 10.1016/j.cej.2018.04.161 [17] CANTRELL K B, HUNT P G, UCHIMIYA M, et al. Impact of pyrolysis temperature and manure source on physicochemical characteristics of biochar[J]. Bioresource Technology,2012,107:419-428. doi: 10.1016/j.biortech.2011.11.084 [18] YUN H, LIANG B, KONG D Y, et al. Improving biocathode community multifunctionality by polarity inversion for simultaneous bioelectroreduction processes in domestic wastewater[J]. Chemosphere,2018,194:553-561. doi: 10.1016/j.chemosphere.2017.12.030 [19] YAO M C, DUAN L, WEI J, et al. Carbamazepine removal from wastewater and the degradation mechanism in a submerged forward osmotic membrane bioreactor[J]. Bioresource Technology,2020,314:123732. doi: 10.1016/j.biortech.2020.123732 [20] CHEN M, ZHOU X F, YU Y Q, et al. Light-driven nitrous oxide production via autotrophic denitrification by self-photosensitized Thiobacillus denitrificans[J]. Environment International,2019,127:353-360. doi: 10.1016/j.envint.2019.03.045 [21] TIAN X M, SHEN Z Q, ZHOU Y X, et al. Inhibition on biological acidification and microbial community by high-strength acetaldehyde[J]. Process Safety and Environmental Protection,2020,143:231-238. doi: 10.1016/j.psep.2020.07.001 [22] GUSTAVE W, YUAN Z F, SEKAR R, et al. Relic DNA does not obscure the microbial community of paddy soil microbial fuel cells[J]. Research in Microbiology,2019,170(2):97-104. doi: 10.1016/j.resmic.2018.11.002 [23] ZHU C Y, WANG H L, YAN Q, et al. Enhanced denitrification at biocathode facilitated with biohydrogen production in a three-chambered bioelectrochemical system (BES) reactor[J]. Chemical Engineering Journal,2017,312:360-366. doi: 10.1016/j.cej.2016.11.152 [24] WU L N, SHEN M Y, LI J, et al. Cooperation between partial-nitrification, complete ammonia oxidation (comammox), and anaerobic ammonia oxidation (anammox) in sludge digestion liquid for nitrogen removal[J]. Environmental Pollution,2019,254:112965. ⊗ doi: 10.1016/j.envpol.2019.112965