Mercury oxidation coupled to autotrophic denitrifying branched sulfur oxidation and sulfur disproportionation for simultaneous removal of Hg0 and NO.

Coupling elemental mercury (Hg0) oxidation, autotrophic denitrifying sulfur oxidation, and sulfur disproportionation offers technological potential for simultaneous Hg0 and nitric oxide (NO) removal. This study shed light on simultaneous demercuration and denitration of flue gas by a sulfur-oxidizing membrane biofilm reactor (MBfR). Removal efficiency of Hg0 and NO attained 92% and 83%, respectively in long-term operation. Taxonomic and metagenomic study revealed that a tremendous variety of Hg0-oxidizing bacteria (MOB) (Thiobacillus, Truepera, etc.), denitrifying/sulfur-oxidizing bacteria (DSOB) (Thioalkalivibrio, Thauera, etc.), sulfur-disproportionating bacteria (SDB) (Desulfobulbus, Desulfomicrobium, etc.), and multi-functional bacteria (Halothiobacillus, Thiobacillus, etc.) significantly increased in abundance during growth under feeding of Hg0 and NO in simulated flue gas. The comprehensive employment of sequential chemical extraction processes, inductive coupled mass spectrometry, X-ray diffraction, X-ray photoelectron spectroscopy, and scanning electron microscopy coupled to energy disperse spectroscopy confirmed that Hg0 was finally biologically oxidized to crystallized metacinnabar (ß-HgS) extracellular micromolecular particles. Our findings provided mechanistic insights that MOB, DSOB, and multi-functional bacteria synergistically bio-oxidized Hg0 as the initial electron donor to Hg2+ and denitrified NO as the terminal electron acceptor to N2. SDB disproportionated S0 branched from S2O32- into S2- and SO42-, and ß-HgS formation from Hg2+ and disproportionation-derived S2-, thermodynamically favored Hg0 bio-oxidation. This novel biotechnique can be a cost-effective and environmentally friendly alternative to flue gas Hg0 and NO treatment. KEY POINTS: • Combination of Hg0 bio-oxidation and autotrophic denitrifying sulfur oxidation achieved simultaneous Hg0 and NO removal. • Thiosulfate disproportionation reinforced Hg0 bio-oxidation for Hg0 removal. • Mercury-oxidizing bacteria, denitrifying/sulfur-oxidizing bacteria, and sulfur-disproportionating bacteria synergistically accomplished Hg0 and NO removal.

Bioconversion of Hg0 into HA-Hg for simultaneous removal of Hg0 and NO in a denitrifying membrane biofilm reactor.

Bacterial mercury oxidation coupled to denitrification offers great potential for simultaneous removal of elemental mercury (Hg0) and nitric oxide (NO) in a denitrifying membrane biofilm reactor (MBfR). Four potentially contributory mechanisms tested separately, namely, membrane gas separation, medium absorption, biosorption and biotransformation, which contributed 4.9%/7.2%, 8.1%/8.9%, 38.8%/9.5% and 48.2%/84.9% of overall Hg0/NO removal in MBfR. Herein, Hg0 bio-oxidation, oxidative Hg0 biosorption and denitrification played leading roles in simultaneous removal of Hg0 and NO. Living microbes performed simultaneous Hg0 bio-oxidation and denitrification, in which Hg0 as electron donor was biologically oxidized to oxidized mercury (Hg2+), while NO as the terminal electron acceptor was denitrified to N2. The Hg2+ further complexed with humic acids in extracellular polymeric substances via functional groups (-SH, -OH, -NH- and -COO-) and formed humic acids bound mercury (HA-Hg). Non-living microbial matrix performed oxidative Hg0 biosorption, in which Hg0 may be physically adsorbed by cellular matrix, then non-metabolically oxidized to Hg2+ via oxidative complexation with -SH in humic acids and finally cleavage of S-H bond and surface charge transfer led to formation of HA-Hg. Therefore, bioconversion of Hg0 to HA-Hg by Hg0 bio-oxidation and oxidative Hg0 biosorption coupled with NO denitrification to N2 dynamically cooperated to accomplish simultaneous removal of Hg0 and NO in MBfR.

Photocatalytic membrane combined with biodegradation for toluene oxidation.

Photocatalytic membrane coupled to biodegradation offers potential for degrading volatile organic compounds (VOCs) in photocatalytic membrane biofilm reactor. An intimately coupled photocatalysis and biodegradation reactor was operated in continuous operation for 500 days to treat simulated waste gas containing toluene. Toluene removal efficiency obtained 99%, with the elimination capacity of 550 g m-3·h-1. Membrane photocatalysis coupled to biodegradation was created to improve toluene removal from 11 to 20%. The dominant genera were Lysinibacillus, Hydrogenophaga, Pseudomonas at 30 d, Rudaea, Dongia, Litorilinea at 230 d xyl, Tod, Tcb, Bed, Tmo, Tbu, Tou, Dmp, Cat were functional genes of toluene metabolism, as shown by16S rDNA and metagenomic sequencing. Photocatalysis destroyed part of the toluene into biodegradable intermediates that were immediately mineralized by microorganisms in biofilm, some toluene was directly degraded by toluene degrading bacterial community into carbon dioxide and water. The novel hybrid photocatalytic membrane biofilm reactor is a cost-effective and robust alternative to VOCs treatment.

Simultaneous mercury oxidation and NO reduction in a membrane biofilm reactor.

This work demonstrates bacterial oxidation of mercury (Hg0) coupled to nitric oxide (NO) reduction in a denitrifying membrane biofilm reactor (MBfR). In 93 days' operation, Hg0 and NO removal efficiency attained 90.7% and 74.1%, respectively. Thauera, Pseudomonas, Paracoccus and Pannonibacter played dual roles as Hg0 oxidizers and denitrifiers simultaneously. Denitrifying bacteria and the potential mercury resistant bacteria dominated the bacterial community. Denitrification-related genes (norB, norC, norD, norE, norQ and norV) and enzymatic Hg0 oxidation-related genes (katG, katE) were responsible for bacterial oxidation of Hg0 and NO reduction, as shown by metagenomic sequencing. XPS, HPLC-ICP-MS and SEM-EDS indicated the formation of a stable mercuric species (Hg2+) reasulting from Hg0 oxidation in the biofilm. Bacterial oxidation of Hg0 was coupled to NO reduction in which Hg0 served as the initial electron donor while NO served as the terminal electron acceptor and thereby redox between Hg0 and NO was formed. MBfR was capable of both Hg0 bio-oxidation and denitrifying NO reduction. This research opens up new possibilities for application of MBfR to simultaneous flue gas demercuration and denitration.

Removal of dimethyl sulfide by the combination of non-thermal plasma and biological process.

A bench scale system integrated with a non-thermal plasma (NTP) and a biotricking filtration (BTF) unit for the treatment of gases containing dimethyl sulfide (DMS) was investigated. DMS removal efficiency in the integrated system was up to 96%. Bacterial communities in the BTF were assessed by PCR-DGGE, which play the dominant role in the biological processes of metabolism, sulfur oxidation, sulfate-reducing and carbon oxidation. The addition of ozone from NTP made microbial community in BTF more complicated and active for DMS removal. The NTP oxidize DMS to simple compounds such as methanol and carbonyl sulfide; the intermediate organic products and DMS are further oxidized to sulfate, carbon dioxide, water vapors by biological degradation. These results show that NTP-BTF is achievable and open new possibilities for applying the integrated with NTP and BTF to odour gas treatment.