Conventional sulfur autotrophic denitrification (SAD) is constrained by effluent acidification and inability to remove phosphorus, while the resource utilization of coal gangue (CG), a massive solid waste, remains challenging. To address both issues, this study developed a novel composite filler by integrating elemental sulfur (S0) with CG and established a coal gangue-based sulfur autotrophic denitrification (CGSAD) biofilter. The system was comprehensively evaluated across various hydraulic retention times (HRT: 0.5–4 h) and temperatures (10–30 °C). During 132 d of operation, CGSAD maintained an average NO3−-N removal efficiency of 82.86% even at a short HRT of 1 h. It demonstrated superior low-temperature adaptability, removing 77.27% of NO3−-N and 53.87% of PO43−-P at 10 °C, significantly outperforming conventional SAD. Phosphorus was mainly removed via metal-phosphate precipitation, driven by H+ released from autotrophic denitrification that promoted metal dissolution from CG and subsequent precipitation, as verified by SEM-EDS. Sulfur-oxidizing bacteria (e.g., Thiobacillus, Sulfurimonas) were highly enriched as core functional genera. Metagenomic and microbial community analyses confirmed the enrichment of key functional genes and the formation of a resilient biofilm with abundant extracellular polymeric substances, supporting system stability under low-temperature stress. The CGSAD system also exhibited effective pH self-buffering without external alkalinity supplementation. Overall, this process provides a sustainable and efficient solution for simultaneous N and P removal from low C/N wastewater, enabling resource utilization of coal gangue while overcoming key bottlenecks of traditional SAD.
| [1] |
Bahgat N T , Siddiqui A , Wilfert P , Korving L , van Loosdrecht M C M . (2024). FePO4. 2H2O recovery from acidic phosphate-rich waste streams. Water Research, 260: 121905
|
| [2] |
Britschgi L , Wei S , Proesl A , Morgenroth E , Derlon N . (2025). The critical role of flocs in nitrification in full-scale aerobic granular sludge-based WWTP. Water Research, 274: 123021
|
| [3] |
Chen R X , Zhao Q , Wang L Y , Zhang Q , Li X Y , Peng Y Z . (2026). Novel dual-particle sulfur-driven partial denitrification coupled with anammox for robust nitrogen removal at ambient temperature. Engineering Environment, 20(1): 13
|
| [4] |
Cheng Y , Li H B , He W J , Dong H , Wang L F , Guo G , Chen G H , Ma J . (2025a). Novel strategy for recovering phosphorus from sulfate-rich wastewater combined with phosphogypsum recycling. Bioresource Technology, 435: 132861
|
| [5] |
Cheng Y , Ren H L , Koju R , Li H Y , Hu C Z . (2025b). Promotion for deep denitrification and sludge minimization by enhancing sulfur-driven endogenous carbon release and electron transport. Chemical Engineering Journal, 520: 165833
|
| [6] |
Cui P , Wan N H , Li C Y , Zou L , Ma M , Du J , Jiang Y . (2024). Comparative analysis of sulfur-driven autotrophic denitrification for pilot-scale application: pollutant removal performance and metagenomic function. Bioresource Technology, 413: 131433
|
| [7] |
Dang X Y , Li X , Zhao C Y , Zhang Y P , Gao X L , He S M , Han J , Zhu Y N , Wang Y Z , Zhu T . (2025). Impact of temperature switching on nitrogen removal and effluent S/N ratio via sulfur autotrophic denitrification. Biochemical Engineering Journal, 219: 109703
|
| [8] |
Du P , Ren Y G , Liu Z F , He J J , Wang L T . (2025). From waste to resources: coal gangue utilization: a comprehensive analysis. Process Safety and Environmental Protection, 201: 107558
|
| [9] |
Fang J L , Wang Y , Wang B Z , Hu H X , Feng Z H , Zhong H Y , Li J . (2025b). Comparative advantages of biogenic sulfur over chemical elemental sulfur as electron donors in sulfur-driven autotrophic denitrification: denitrification performance, sludge characteristics and microbial responses. Journal of Environmental Chemical Engineering, 13(5): 117721
|
| [10] |
Fang Y , Huang R T , Zhang Y Y , Zhang J , Xi W N , Shi X Y . (2025a). Utilizing machine learning models to grasp water quality dynamic changes in lake eutrophication through phytoplankton parameters. Frontiers of Environmental Science & Engineering, 19(2): 14
|
| [11] |
Ge S J , Chen G , Yuan L M , Lv J , Shi T T , Zhang C Y . (2026). Simultaneous denitrification and phosphorus removal accomp-lished by denitrifying biofilters assembled with innovative sulphur-fly ash ceramic carriers. Journal of Environmental Management, 397: 128334
|
| [12] |
Gu C K , Li X Y , Zhang S J , Li J W , Gao X Y , Chen G , Wang Z B , Peng Y Z . (2024). Advanced nitrogen and phosphorus removal in pilot-scale anaerobic/aerobic/anoxic system for municipal wastewater in Northern China. Bioresource Technology, 399: 130616
|
| [13] |
Guo H L , Wang S Y , Zhu C Y , Chang J S , Lee D J . (2025). Exceptional nitrate and phosphate removals from low carbon-to-nitrogen ratio wastewater with a novel pyrite-sulfur composite filler. Process Safety and Environmental Protection, 203: 107941
|
| [14] |
Guo Q , Li H L , Fu M B , Li Y L , Tian D C , Zhang L . (2023). Enhanced hydrolysis of aluminum nitride from secondary aluminum dross through combination of wet-stirred milling and alkaline leaching. Waste and Biomass Valorization, 14(12): 4257–4268
|
| [15] |
Hou M X , Gu X S , Lai W Y , Fan Y Y , Sun S S , Yan P , Zhang Y , Zheng X Y , He S B . (2025). Sulfur-iron interactions forming activated FexSy pool in-situ to synergistically improve nitrogen removal in denitrification system. Journal of Environmental Management, 388: 126047
|
| [16] |
Hu K Y , Liu X M , Jia X , Zhang Z H , Liu W Q , Li J , Yao X R . (2026). Advances in sulphur-iron autotrophic denitrification research and exploration of its future application in wastewater treatment: a critical review. Bioresource Technology, 439: 133391
|
| [17] |
Huang G D , Ji Y S , Li J , Hou Z H , Dong Z C . (2018). Improving strength of calcinated coal gangue geopolymer mortars via increasing calcium content. Construction and Building Materials, 166: 760–768
|
| [18] |
Jung H , Kim J , Lee J . (2025). Seasonal and spatial contributions of sulfate and trace elements in river water in mining districts: insights from hydrogeochemical and isotopic analysis based on statistical models. Journal of Hazardous Materials, 488: 137246
|
| [19] |
Kang L , Xu B Y , Li P F , Wang K , Chen J , Du H L , Liu Q Q , Zhang L , Lian X Q . (2025). Controllable preparation of low-cost coal gangue-based SAPO-5 molecular sieve and its adsorption performance for heavy metal ions. Nanomaterials, 15(5): 366
|
| [20] |
Li X L , Sun H W , Li Z T , Yang X Y , Wang G , Zhang Y X , Liu Y C . (2025). Kanamycin promoted the enrichment of comammox Nitrospira from aerobic-activated sludge. Journal of Environmental Chemical Engineering, 13(2): 115900
|
| [21] |
Li X Y , Shao J H , Zheng J Q , Bai C Y , Zhang X H , Qiao Y J , Colombo P . (2023). Fabrication and application of porous materials made from coal gangue: a review. International Journal of Applied Ceramic Technology, 20(4): 2099–2124
|
| [22] |
Liang N , Qaisar M , Zhang K Y , Zhu X P , Cai J . (2025). A novel phosphorus removal process in the sulfide-based autotrophic denitrification system. Journal of Environmental Chemical Engineering, 13(1): 115268
|
| [23] |
Liao X X , Qian J S , Shi Y J , Yang L Y , Chen X M . (2025). Distinct fate of hydrazine in sulfur-driven autotrophic denitrification. Chemical Engineering Journal, 522: 167308
|
| [24] |
Liu Q T , Du R , Fan J R , Peng Y Z . (2026). Linking nitrite accumulation to shift in carbon utilization of denitrification: from single to composite electron donor. Engineering Environment, 20(2): 19
|
| [25] |
Liu X ZZhao C SXu T TLiu WChen Q FLi L ZTan YWang X KDong Y N (2023). Pyrite and sulfur-coupled autotrophic denitrification system for efficient nitrate and phosphate removal. Bioresource Technology, 384: 129363
|
| [26] |
Lu H , Huang H Q , Yang W M , Mackey H R , Khanal S K , Wu D , Chen G H . (2018). Elucidating the stimulatory and inhibitory effects of dissolved sulfide on sulfur-oxidizing bacteria (SOB) driven autotrophic denitrification. Water Research, 133: 165–172
|
| [27] |
Lv L Y , Feng C D , Li W G , Ren Z J , Wang P F , Liu X Y , Gao W F , Sun L , Zhang G M . (2023). Accelerated performance recovery of anaerobic granular sludge after temperature shock: rapid construction of protective barriers (EPS) to optimize microbial community composition base on quorum sensing. Journal of Cleaner Production, 392: 136243
|
| [28] |
Miao H H , Zeng W , Li J M , Liu H , Zhan M J , Dai H X , Peng Y Z . (2022). Simultaneous nitrate and phosphate removal based on thiosulfate-driven autotrophic denitrification biofilter filled with volcanic rock and sponge iron. Bioresource Technology, 366: 128207
|
| [29] |
(2024). . , 62: 10257
|
| [30] |
Preetham V , Saidulu D , Tiwary C S , Gupta A K . (2026). Role of biofilm activity on novel interwoven lattice-shaped 3D printed biocarrier for enhanced removal of organics and nutrients with reduced footprint: performance assessment and microbial community dynamics. Bioresource Technology, 439: 133356
|
| [31] |
Ren D H , Zuo Z Q , Ba X C , He W K , Yuan S K , Cen Y X , Zhang G J , Xu J M , Zhang N , Sun Y L . et al. (2025). Fe(Ⅱ/Ⅲ) cycling-based buffering strategy to mitigate sulfide and nitrate overflow in sulfur autotrophic denitrification process under wastewater quality fluctuations. Water Research, 286: 124243
|
| [32] |
Shi Y S , Pang B Y , Jia Y Y , Zheng Z N , Quan H T , Qi P , Hao T W , Sun L P , Lu H . (2026). Enhancing nitrogen removal in low C/N wastewater via carbon resource recovery from biochar-mediated anaerobic digestion of discarded cefradine residues. Water Research, 288: 124641
|
| [33] |
Sivabalasarma S , Taib N , Mollat C L , Joest M , Steimle S , Gribaldo S , Albers S V . (2025). Structure of a functional archaellum in Bacteria of the Chloroflexota phylum. Nature Microbiology, 10(10): 2412–2424
|
| [34] |
State Administration for Market RegulationNational Standardization Administration (2023). Standards for Drinking Water Quality GB 5749–2022. Beijing: Standard Press of China
|
| [35] |
Su Z A , Zhao J T , Lu Z , Wang M D , Guo C C , Song X , Guo X B , Cai M , Wu Z J . (2022). The effects of different temperature conditions on sludge characteristics and microbial communities of nitritation denitrification. Journal of Water Process Engineering, 50: 103283
|
| [36] |
Sun J L , Li H Y , Dong H , Liu L , Zhou C Y , Du Z W , Dang Y , Holmes D E . (2025). Magnetite-augmented sulfur-siderite autotrophic denitrification: deep nitrogen removal at ultra-low HRT from lab to pilot scale. Water Research, 284: 124034
|
| [37] |
Tang W T , Xiao Y H , Deng Y F , Tan Y K , Chen G H , Hao T W . (2024). Model and experiment-based evaluation of seawater-based urine phosphorus recovery (SUPR) process. Frontiers of Environmental Science & Engineering, 18(11): 141
|
| [38] |
Wan D J , Li Q , Liu Y D , Xiao S H , Wang H J . (2019). Simultaneous reduction of perchlorate and nitrate in a combined heterotrophic-sulfur-autotrophic system: secondary pollution control, pH balance and microbial community analysis. Water Research, 165: 115004
|
| [39] |
Wang F , Li J , Duan H L . (2022). A sulfur-limestone bioretention system for stormwater treatment: nitrogen removal performance and microbial community. Science of the Total Environment, 827: 154301
|
| [40] |
Wang W , Wei D Y , Li F C , Zhang Y W , Li R H . (2019). Sulfur-siderite autotrophic denitrification system for simultaneous nitrate and phosphate removal: from feasibility to pilot experiments. Water Research, 160: 52–59
|
| [41] |
Wen X Z , Qu F T , Chen J R , Tao W Y , Zhou J , Yang H Y , Wei Z M . (2025). Evaluation of coal gangue resource utilization: a study on the humification process and microbial community dynamics in composting with different particle sizes of coal gangue. Process Safety and Environmental Protection, 202: 107701
|
| [42] |
WHO (2022). Guidelines for Drinking-water Quality: Fourth Edition Incorporating the First and Second Addenda. Geneva: World Health Organization
|
| [43] |
Xu F , Peng Y Y , Gu X S , Sun S S , Li A Q , He S B . (2024). Revealing sulfur-iron coupling mechanism for enhanced autotrophic denitrification in ecological floating beds. Bioresource Technology, 402: 130800
|
| [44] |
Xu J M , Sun Y L , Yao X D , Zhang G J , Zhang N , Wang H C , Wang S S , Wang A J , Cheng H Y . (2023). Highly efficient coremoval of nitrate and phosphate driven by a sulfur-siderite composite reactive filler toward secondary effluent polishing. Environ-mental Science & Technology, 57(43): 16522–16531
|
| [45] |
Xu W J , He Y Y , Cheng F Q . (2025). Mutual remediation of CO2 emissions and industrial wastewater: feasibility, application, and ecological impact. Frontiers of Environmental Science & Engineering, 19(6): 84
|
| [46] |
Yang X L , He Y Y , Liu Y R , Wang H W , Zhang P Y , Zhu T T , Wang Y F , Zhao Y X , Tong Y D , Chen X M . et al. (2025). Mechanisms and mitigation strategies of N2O emission in response to metal nanoparticles in wastewater treatment: a review. Journal of Cleaner Production, 520: 146190
|
| [47] |
Yuan S W , Xu Y P , Wang P F , Xie R L , Hu J B , Fu Z H , Wang K , Wang S H , Jiang X , Rao K F . et al. (2025). Characterizing molecular fingerprint of dissolved organic matter shaped by natural and anthropogenic factors in a large macrophytic shallow lake wetland. Frontiers of Environmental Science & Engineering, 19(3): 31
|
| [48] |
Zhang C Y , Zhu Z P , Yuan L M , Yang D X , Xu Q , Ge S J . (2025a). Insights into seasonal temperature shifts on a robust composite-substrate autotrophic denitrification reactor for treating municipal secondary effluent. Frontiers of Environmental Science & Engineering, 19(6): 82
|
| [49] |
Zhang S R , Tang Z C , Xu X W , Jiang Y X , Guo J S , Fang F . (2025b). Effects of the coexistence of polystyrene microplastics and imidacloprid on nitrogen and phosphorus transformation in soil. Frontiers of Environmental Science & Engineering, 19(2): 15
|
| [50] |
Zhang Y , Li M Q , Dong L , Han C X , Li M , Wu H M . (2021). Effects of biochar dosage on treatment performance, enzyme activity and microbial community in aerated constructed wetlands for treating low C/N domestic sewage. Environmental Technology & Innovation, 24: 101919
|
| [51] |
Zhang Z , Zhang C H , Yang Y , Zhang Z W , Tang Y H , Su P D , Lin Z W . (2022). A review of sulfate-reducing bacteria: Metabolism, influencing factors and application in wastewater treatment. Journal of Cleaner Production, 376: 134109
|
| [52] |
Zhao Q , Wang L Y , Jia T P , Li X Y , Zhang Q , Peng Y Z . (2024). Elemental sulfur-siderite composite filler empowers sustainable tertiary treatment of municipal wastewater even at an ultra-low temperature of 7.3 °C. Nature Water, 2(8): 782–792
|
| [53] |
Zheng R , Zhang K , Kong L R , Liu S T . (2024). Research progress and prospect of low-carbon biological technology for nitrate removal in wastewater treatment. Frontiers of Environmental Science & Engineering, 18(7): 80
|
| [54] |
Zhou K B , Zhang H , Guo D , Gao S C , Pei Y S , Hou L . (2024). Amorphous Fe substrate enhances nitrogen and phosphorus removal in sulfur autotrophic process. Water Research, 256: 121581
|
| [55] |
Zhu X B , Gong W H , Li W , Bai X Y , Zhang C X . (2022). Reclamation of waste coal gangue activated by Stenotrophomonas maltophilia for mine soil improvement: solubilizing behavior of bacteria on nutrient elements. Journal of Environmental Management, 320: 115865
|
RIGHTS & PERMISSIONS
Higher Education Press 2026