Structure-activity relationship between crystal plane and pyrite-driven autotrophic denitrification efficacy: Electron transfer and metagenome-based microbial mechanism

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Water Research Pub Date : 2024-11-05 DOI:10.1016/j.watres.2024.122756

Yingmu Wang , Shi Chen , Yuanjing Chen , Junge Xu , Jian Zhou , Qiang He , Ziyuan Lin , Kai-qin Xu , Gongduan Fan

{"title":"Structure-activity relationship between crystal plane and pyrite-driven autotrophic denitrification efficacy: Electron transfer and metagenome-based microbial mechanism","authors":"Yingmu Wang , Shi Chen , Yuanjing Chen , Junge Xu , Jian Zhou , Qiang He , Ziyuan Lin , Kai-qin Xu , Gongduan Fan","doi":"10.1016/j.watres.2024.122756","DOIUrl":null,"url":null,"abstract":"<div><div>Pyrite-driven autotrophic denitrification (PAD) has been recognized as a promising treatment technology for nitrate removal. Although the occurrence of PAD has been found in recent years, there is a knowledge gap about effects of crystal plane of pyrite on the performance and mechanism of PAD system. Here, this study investigated the effects of crystal planes ({100}, {111} and {210}) of single-crystal pyrite on denitrification performance, electron transfer, and microbial mechanism in PAD system. The removal efficiency of nitrate in B-{210} reached 100%, which was 1.67-fold and 2.86-fold higher than that of B-{100} and B-{111}, respectively. X-ray photoelectron spectroscopy and electrochemical results indicated that Fe-S bonds of pyrite with {210} crystal plane were more susceptible to breakage by Fe3+ oxidation assault, and leaching microbially available Fe2+ and sulfur intermediates to drive autotrophic denitrification. Metagenomic results suggested that community of functional pyrite-driven denitrifiers varied in response to crystal plane, and abundances of N-S transformation and EET-related microbes and genes in B-{210} notably up-regulated compared to B-{100} and B-{111}. In addition, this work proposed a dual-mode for electron transfer pathway during pyrite oxidation and nitrogen transformation in PAD system. In B-{210}, Fe(II)- and sulfur-driven denitrifiers obtained electron after pyrite oxidation-dissolution, and the enrichment of pyrite-oxidizing bacteria in B-{210} could enhance the electron transfer from pyrite through electron shuttles. This work highlighted that stronger surface reactivity and electron shuttle effect in B-{210} enhanced electron transfer, leading to favorable PAD performance in B-{210}. Overall, this study provides novel insights into the structure-activity relationship between the crystal plane structure of pyrite and denitrification activity in PAD system.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"268 ","pages":"Article 122756"},"PeriodicalIF":11.4000,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Water Research","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0043135424016555","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}

引用次数: 0

Abstract

Pyrite-driven autotrophic denitrification (PAD) has been recognized as a promising treatment technology for nitrate removal. Although the occurrence of PAD has been found in recent years, there is a knowledge gap about effects of crystal plane of pyrite on the performance and mechanism of PAD system. Here, this study investigated the effects of crystal planes ({100}, {111} and {210}) of single-crystal pyrite on denitrification performance, electron transfer, and microbial mechanism in PAD system. The removal efficiency of nitrate in B-{210} reached 100%, which was 1.67-fold and 2.86-fold higher than that of B-{100} and B-{111}, respectively. X-ray photoelectron spectroscopy and electrochemical results indicated that Fe-S bonds of pyrite with {210} crystal plane were more susceptible to breakage by Fe³⁺ oxidation assault, and leaching microbially available Fe²⁺ and sulfur intermediates to drive autotrophic denitrification. Metagenomic results suggested that community of functional pyrite-driven denitrifiers varied in response to crystal plane, and abundances of N-S transformation and EET-related microbes and genes in B-{210} notably up-regulated compared to B-{100} and B-{111}. In addition, this work proposed a dual-mode for electron transfer pathway during pyrite oxidation and nitrogen transformation in PAD system. In B-{210}, Fe(II)- and sulfur-driven denitrifiers obtained electron after pyrite oxidation-dissolution, and the enrichment of pyrite-oxidizing bacteria in B-{210} could enhance the electron transfer from pyrite through electron shuttles. This work highlighted that stronger surface reactivity and electron shuttle effect in B-{210} enhanced electron transfer, leading to favorable PAD performance in B-{210}. Overall, this study provides novel insights into the structure-activity relationship between the crystal plane structure of pyrite and denitrification activity in PAD system.

Abstract Image

查看原文

微信好友朋友圈 QQ好友复制链接

本刊更多论文

晶体平面与黄铁矿驱动的自养反硝化功效之间的结构-活性关系：电子传递和基于元基因组的微生物机制

黄铁矿驱动的自养反硝化（PAD）被认为是一种很有前景的硝酸盐去除处理技术。虽然近年来发现了黄铁矿自养反硝化现象，但关于黄铁矿晶面对自养反硝化系统性能和机理的影响还存在知识空白。本研究探讨了单晶黄铁矿的晶面（{100}、{111}和{210}）对 PAD 系统中脱硝性能、电子传递和微生物机理的影响。B-{210}对硝酸盐的去除率达到100%，分别是B-{100}和B-{111}的1.67倍和2.86倍。X射线光电子能谱和电化学结果表明，{210}晶面的黄铁矿的Fe-S键更容易被Fe3+氧化作用破坏，并浸出微生物可利用的Fe2+和硫中间产物，从而驱动自养反硝化作用。元基因组学结果表明，黄铁矿驱动的功能性反硝化菌群落随晶面的变化而变化，与B-{100}和B-{111}相比，B-{210}中N-S转化和EET相关微生物和基因的丰度明显上调。此外，这项研究还提出了PAD系统中黄铁矿氧化和氮转化过程中电子传递途径的双重模式。在B-{210}中，铁（II）和硫驱动的反硝化菌在黄铁矿氧化溶解后获得电子，而B-{210}中黄铁矿氧化菌的富集可通过电子穿梭器加强黄铁矿的电子传递。这项工作突出表明，B-{210}中更强的表面活性和电子穿梭效应增强了电子传递，从而使B-{210}具有良好的PAD性能。总之，本研究为黄铁矿晶体平面结构与 PAD 系统中脱硝活性之间的结构-活性关系提供了新的见解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文去求助

来源期刊

Water Research 环境科学-工程：环境

CiteScore

20.80

自引率

9.40%

发文量

1307

审稿时长

38 days

期刊介绍： Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.