Bioresource Technology 249 (2018) 844–850
Total Page：16
File Type：pdf, Size：1020Kb
Bioresource Technology 249 (2018) 844–850 Contents lists available at ScienceDirect Bioresource Technology journal homepage: www.elsevier.com/locate/biortech Accelerated removal of high concentration p-chloronitrobenzene using MARK bioelectrocatalysis process and its microbial communities analysis ⁎ Xinhong Penga,b, , Xianhui Pana, Xin Wangb, Dongyang Lia, Pengfei Huanga, Guanhua Qiua, Ke Shana, Xizhang Chua a Institute of Seawater Desalination and Multipurpose Utilization, State Oceanic Administration (SOA), Nankai District, Tianjin 300192, China b MOE Key Laboratory of Pollution Processes and Environmental Criteria, Tianjin Key Laboratory of Environmental Remediation and Pollution Control, Nankai University, No. 38 Tongyan Road, Jinnan District, Tianjin 300350, China ARTICLE INFO ABSTRACT Keywords: p-Chloronitrobenzene (p-CNB) is a persistent refractory and toxic pollutant with a concentration up to 200 mg/L Bio-electrocatalysis in industrial wastewater. Here, a super-fast removal rate was found at 0.2–0.8 V of external voltage over a p-CNB p-Chloronitrobenzene concentration of 40–120 mg/L when a bioelectrochemical technology is used comparing to the natural biode- Initial concentration gradation and electrochemical methods. The reduction kinetics (k) was fitted well according to pseudo-first Applied voltage order model with respect to the different initial concentration, indicating a 1.12-fold decrease from 1.80 to Microbial communities diversity − 0.85 h 1 within the experimental range. Meanwhile, the highest k was provided at 0.5 V with the characteristic of energy saving. It was revealed that the functional bacterial (Propionimicrobium, Desulfovibrio, Halanaerobium, Desulfobacterales) was selectively enriched under electro-stimulation, which possibly processed Cl-substituted nitro-aromatics reduction. The possible degradation pathway was also proposed. This work provides the ben- eficial choice on the rapid treatment of high-concentration p-CNB wastewater. 1. Introduction 2015). Therefore, it is absolutely necessary to seek new, green, and high-efficient approach to accelerate the reductive transformation of p- p-Chloronitrobenzene (p-CNB), a kind of important raw material for CNB to low-toxic compounds. industry synthesis of pesticides, medicines, lumber preservatives, sul- Bio-electrocatalysis conversion, noted as the association of bio-de- phur dyes, pharmaceuticals, gasoline additives and other chemicals gradation and electrochemical catalytic reduction, has recently been (Xia et al., 2011), has the characterization of high persistence in ex- used for successful bioremediation as an innovative, more effective and posed sediments and soil organic material, and poses a critical threat to less expensive wastewater treatment solution for emerging environ- the human health and social safety, due to their mutagenic, carcino- mental issue (Du et al., 2017), and has obvious advantages in con- genic and teratogenic effects resulting from the occurrences of elec- taminant detoxification accompanying with energy saving and con- trophilic nitro and chlorine groups (Li et al., 2015). It is reported that sumption reduction (Puyol et al., 2017), which is significantly against the highest concentration of p-CNB is up to 200 mg/L in industry from the conventional anaerobic and electrochemical processes. At wastewater (Linch, 1974). Thus, p-CNB is listed as precedence-con- present, two main bio-electrocatalytic processes are accepted: microbial trolled organic pollutant by US EPA and EC (Jones et al., 2006). The fuel cell and microbial electrolysis cell. The former is the direct oxi- traditional treatment processes address physical adsorption (Guo and dation/reduction of recalcitrant wastes by bio-catalysis with self-driven Zheng, 2009), advanced oxidization conversion (Li and Zhu, 2014; Ye electrostimulation, for example, Fan et al. successfully enhanced the et al., 2010; Yuan et al., 2012) and biological degradation (Alatraktchi removal of tetrabromobisphenol by anodic anaerobic co-metabolic et al., 2014; Xia et al., 2011). However, physicochemical methods are biodegradation using biocatalytic fuel cell (Fan et al., 2017). Miran usually marked as a pre-treatment to enhance the biodegradability of et al. achieved azo dye degradation by cathodic bio-reduction in dual recalcitrant wastewater with the disadvantage of high energy demands chamber microbial fuel cell (Miran et al., 2015). The other is to degrade and capital costs (Hurwitz et al., 2014), whose viability requires to be the contaminant on the base of the reduction of energy barrier by virtue further improved. The bio-treatment technology is usually extremely of external electrostimulation. It has been confirmed to be feasible time-consuming under anaerobic condition (Dareioti and Kornaros, to applied in the removal of substituted aromatic compounds by ⁎ Corresponding author at: Institute of Seawater Desalination and Multipurpose Utilization, State Oceanic Administration (SOA), Nankai District, Tianjin 300192, China. E-mail address: [email protected] (X. Peng). http://dx.doi.org/10.1016/j.biortech.2017.10.068 Received 13 July 2017; Received in revised form 9 October 2017; Accepted 18 October 2017 Available online 19 October 2017 0960-8524/ © 2017 Elsevier Ltd. All rights reserved. X. Peng et al. Bioresource Technology 249 (2018) 844–850 biocathode electrolysis technique, such as p-fluoronitrobenzene (Shen ionization (EI) ion source of 70 eV and a HP-5MS capillary column et al., 2014), chloramphenicol (Kong et al., 2014a), p-nitrophenol (Tao (30 m × 250 μm × 0.25 μm). The GC injection and interface ports were et al., 2013), azo dye (Wang et al., 2016) and so on. It was studied that set at 250 °C and 280 °C, respectively, with an injection volume of 1 μL the bio-electrocatalysis conversion process could facilitate the p-CNB at a constant flow rate of 1 mL/min. The GC oven temperature program removal (Guo et al., 2015). However, its reduction rate was relatively was as follows: held at 35 °C for 2 min; increased up to 150 °C for 1 min − low with the value of 0.2291 h 1 only for 20 mg/L p-CNB. at 10 °C/min; and then increased up to 280 °C for 5 min at 20 °C/min. In this work, p-CNB with higher concentration up to 120 mg/L had According to the results of qualitative analysis by GC, the pollutant been rapidly degraded with higher reduction kinetics by the bio-elec- and its transformation products (p-chloroaniline (p-CAN) and aniline trocatalysis process using an adjusting architecture. The effect of initial (AN)) were quantified by the calibration curve of the pure compounds pollutant concentrations (40–120 mg/L) and applied external voltage relative to external standards at 275 nm for p-CNB, 240 nm for p-CAN (0–0.8 V) on p-CNB reduction rates was taken into account. At the and 231 nm for AN using high performance liquid chromatography meantime, it is known that the bio-electrocatalytic process is extra- (HPLC, Agilent 1200 series, Agilent, USA), respectively, which complicated. Based on the analysis of microbial communities structure, equipped with a diode array detector (DAD) and a Zorbax Eclipse XDB- the possible degradation pathway and bio-electrochemical analysis C18 reversed-phase column (4.6 mm × 150 mm × 5 μm). The sample were also explored. In addition, the water quality of p-CNB wastewater was mixed (v/v, 1:1) with methanol, and then filter by 0.22 μmmi- before and after treatment was subjected to chemical oxygen demand croporous membrane. The mobile phase was water-methanol (v/v, 4:6) (COD) determination. It is noteworthy that the optimization of opera- with the flow of 1.0 mL/min. The injection volume was 10 μL at the tion condition can lead to cost cutting and high-efficient removal of column temperature of 25 °C. Chemical oxygen demand (COD, TNT target contaminant, thus providing a reference for practical application plus COD Reagent, HACH Company, US) and MLVSS were made ac- of CNBs wastewater treatment. cording to APHA standard methods (APHA, 2005). 2. Materials and methods 2.2.2. Bioelectrochemical technique The voltage across resistor was monitored online every 30 min using 2.1. Experimental construction a date acquisition system (PISO-813, ICP DAS Co. Ltd, China). All the electrode potentials were displayed according to Ag|AgCl|KClsat re- All the rectangular dual chamber reactors, made of the ference electrode (+197 mV vs. standard hydrogen electrode; SHE). polymethyl methacrylate with approximately 4 × 5 × 5 cm3 The bioelectrocatalytical test of cyclic voltammetry (CV) was swept in (height × width × length) were run at 30 ± 0.5 °C temperature-con- situ from 0.6 to −1.0 V (vs. Ag|AgCl|KClsat) at a scan rate of 0.1 mV/s trolled biochemical incubator in fed-batch mode under 10 Ω with DC by a multi-channel potentiostat (CHI1000C, Shanghai CH Instrument power source of 0.5 V except as noted otherwise. Two carbon mesh Company, China) in a three-electrode mode for the configuration re- brush electrodes (3 cm in diameter and 3 cm long) were divided by actor, with the cathode as the working electrode, the anode as the 4×4cm2 (width × length) cation exchange membrane (CEM, Ultrex counter electrode, and an Ag/AgCl close to the cathode as the reference CMI7000, Membranes International Inc., USA) with vertical deploy- electrode. ment. Prior to use, the CEM was equilibrated in 1 M NaCl solution for 24 h. The electrode was subjected to a 24 h acetone soak followed by a 2.2.3. Molecular biotechnique 30 min heat treatment at 450 °C in a muffle furnace, and then adsorbed Bacterial biofilms, sampled by scraping carbon brush carrier using until p-CNB saturation. sterile forceps (Wu et al., 2017), were designed as S0, S1 and S2, which The anode chamber, in the bio-electrocatalytical reactor (BER), was were collected from source inoculum, anaerobic biocarrier and anae- inoculated by the activated sludge from a local sewage treatment plant robic biocathode, respectively. Genome DNA was extracted according in Tianjin City with the mixed liquor volatile suspended solids (MLVSS) to CTAB/SDS method, and confirmed its purity by 1% agarose gel of 3.7 g/L.