{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2025,9,11]],"date-time":"2025-09-11T17:51:18Z","timestamp":1757613078125,"version":"3.44.0"},"reference-count":43,"publisher":"Public Library of Science (PLoS)","issue":"9","license":[{"start":{"date-parts":[[2025,9,4]],"date-time":"2025-09-04T00:00:00Z","timestamp":1756944000000},"content-version":"vor","delay-in-days":0,"URL":"http:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"name":"Guizhou Provincial Science and Technology Projects","award":["No. ZK [2022]328"],"award-info":[{"award-number":["No. ZK [2022]328"]}]},{"name":"Natural Science Foundation of Education Department of Guizhou Province","award":["No. KY [2022]300"],"award-info":[{"award-number":["No. KY [2022]300"]}]},{"name":"Guizhou Science Association Pioneering Project","award":["2025XZQYXM-01-06"],"award-info":[{"award-number":["2025XZQYXM-01-06"]}]},{"name":"Natural Science Foundation of Guizhou Education University","award":["No. 2021BS017"],"award-info":[{"award-number":["No. 2021BS017"]}]}],"content-domain":{"domain":["www.plosone.org"],"crossmark-restriction":false},"short-container-title":["PLoS One"],"abstract":"<jats:p>Antimony (Sb) is extensively utilized in industrial activities, but most of its compounds exhibit human toxicity and are classified as priority-controlled pollutants. Unlike traditional electrochemical methods that remove metallic pollutants via coagulation or precipitation, electrochemical hydride generation technology converts antimony (Sb) in wastewater into stibine gas (SbH<jats:sub>3<\/jats:sub>) for efficient removal. Furthermore, the generated SbH\u2083 can be decomposed thermally to partially recover metallic antimony. In synthetic wastewater treatment (Sb\u2009=\u20095\u2009mg\/L), the proton exchange membrane (Nafion117) electrolysis device achieved an antimony removal efficiency of 72.8\u2009\u00b1\u20092.2%, outperforming traditional cation-exchange membranes. This enhancement is attributed to the membrane\u2019s proton-selective transport and high H conductivity. Increasing the temperature enhanced the generation and release of SbH<jats:sub>3<\/jats:sub>, with the higher removal efficiency of 87.3\u2009\u00b1\u20092.6% achieved at approximately 30 \u00b0C. However, temperatures exceeding 30 \u00b0C could lead to the partial decomposition of SbH<jats:sub>3<\/jats:sub> back into the solution, thereby affecting removal efficiency. Ultrasonic stirring in the cathode chamber significantly enhanced Sb removal from high-concentration solutions (5\u2009mg\/L), while magnetic stirring was more suitable for lower-concentration solutions. Orthogonal experiments revealed that due to the competitive relationship between hydrogen generation and SbH<jats:sub>3<\/jats:sub> generation, as well as the gas-blocking effect, current intensity and electrode area both had a significant impact on Sb removal. Under appropriate current intensity and electrode area conditions (0.5 A, 20 cm\u00b2), a high removal rate of 78.5\u2009\u00b1\u20094.6% can be achieved. Consequently, employing a Nafion membrane coupled with ultrasonic agitation under optimized conditions (30\u00b0C, 25 mA\/cm\u00b2) effectively accelerates antimony removal kinetics and enhances elimination efficiency. However, the substantial reduction in current efficiency and elevated energy consumption induced by competitive hydrogen evolution represent critical challenges requiring urgent resolution. This treatment approach provides a technical reference\u200c for shifting from mere contaminant removal to resource recovery. The integration of removal and recovery processes holds substantial potential\u200c for implementing circular economy models in mining and metallurgical industries.<\/jats:p>","DOI":"10.1371\/journal.pone.0331138","type":"journal-article","created":{"date-parts":[[2025,9,4]],"date-time":"2025-09-04T17:30:06Z","timestamp":1757007006000},"page":"e0331138","update-policy":"https:\/\/doi.org\/10.1371\/journal.pone.corrections_policy","source":"Crossref","is-referenced-by-count":0,"title":["The optimization of electrochemical hydride generation technology for treating antimony-containing wastewater"],"prefix":"10.1371","volume":"20","author":[{"given":"Jingjing","family":"Chen","sequence":"first","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Guoping","family":"Zhang","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Yi","family":"Bai","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Yan","family":"Xiong","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2384-5036","authenticated-orcid":true,"given":"Xing","family":"Liu","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"340","published-online":{"date-parts":[[2025,9,4]]},"reference":[{"key":"pone.0331138.ref001","doi-asserted-by":"crossref","first-page":"125","DOI":"10.1016\/S0012-8252(01)00070-8","article-title":"Antimony in the environment: a review focused on natural waters","volume":"57","author":"M Filella","year":"2002","journal-title":"Earth-Sci Rev"},{"key":"pone.0331138.ref002","doi-asserted-by":"crossref","first-page":"95","DOI":"10.1016\/j.jhazmat.2012.10.005","article-title":"Use of sorbents for purification of lead, copper and antimony in runoff water from small arms shooting ranges","volume":"243","author":"E Mariussen","year":"2012","journal-title":"J Hazard Mater"},{"issue":"9","key":"pone.0331138.ref003","doi-asserted-by":"crossref","DOI":"10.1371\/journal.pone.0183991","article-title":"Effects of antimony on redox activities and antioxidant defence systems in sunflower (Helianthus annuus L.) plants","volume":"12","author":"A Ortega","year":"2017","journal-title":"PLoS One"},{"issue":"2","key":"pone.0331138.ref004","doi-asserted-by":"crossref","DOI":"10.1371\/journal.pone.0229037","article-title":"Bioaccessibility of antimony and other trace elements from lead shot pellets in a simulated avian gizzard environment","volume":"15","author":"AD French","year":"2020","journal-title":"PLoS One"},{"key":"pone.0331138.ref005","doi-asserted-by":"crossref","first-page":"41","DOI":"10.1016\/j.scitotenv.2011.06.009","article-title":"Antimony pollution in China","author":"M He","year":"2012","journal-title":"Sci Total Environ"},{"key":"pone.0331138.ref006","doi-asserted-by":"crossref","first-page":"104528","DOI":"10.1016\/j.apgeochem.2020.104528","article-title":"Antimony mobility during the early stages of stibnite weathering in tailings at the Beaver Brook Sb deposit, Newfoundland","volume":"115","author":"A Bor\u010dinov\u00e1 Radkov\u00e1","year":"2020","journal-title":"Appl Geochem"},{"key":"pone.0331138.ref007","doi-asserted-by":"crossref","first-page":"181","DOI":"10.1016\/j.microc.2017.10.010","article-title":"Environmental geochemical and spatial\/temporal behavior of total and speciation of antimony in typical contaminated aquatic environment from Xikuangshan, China","volume":"137","author":"W Guo","year":"2018","journal-title":"Microchem J"},{"issue":"2","key":"pone.0331138.ref008","doi-asserted-by":"crossref","first-page":"203","DOI":"10.1007\/s11631-019-00382-6","article-title":"Antimony removal from wastewater by sulfate-reducing bacteria in a bench-scale upflow anaerobic packed-bed reactor","volume":"39","author":"J Chen","year":"2019","journal-title":"Acta Geochim"},{"key":"pone.0331138.ref009","doi-asserted-by":"crossref","first-page":"265","DOI":"10.1016\/S0012-8252(02)00089-2","article-title":"Antimony in the environment: a review focused on natural waters","volume":"59","author":"M Filella","year":"2002","journal-title":"Earth-Sci Rev"},{"issue":"1","key":"pone.0331138.ref010","doi-asserted-by":"crossref","DOI":"10.1371\/journal.pone.0114796","article-title":"Sb(V) reactivity with human blood components: redox effects","volume":"10","author":"S L\u00f3pez","year":"2015","journal-title":"PLoS One"},{"key":"pone.0331138.ref011","doi-asserted-by":"crossref","first-page":"34","DOI":"10.1016\/j.aca.2014.11.020","article-title":"Determination of traces of Sb(III) using ASV in Sb-rich water samples affected by mining","volume":"854","author":"R Cidu","year":"2015","journal-title":"Anal Chim Acta"},{"issue":"17","key":"pone.0331138.ref012","doi-asserted-by":"crossref","first-page":"4327","DOI":"10.1016\/j.watres.2009.06.033","article-title":"Removal of antimony(V) and antimony(III) from drinking water by coagulation-flocculation-sedimentation (CFS)","volume":"43","author":"X Guo","year":"2009","journal-title":"Water Res"},{"issue":"3","key":"pone.0331138.ref013","doi-asserted-by":"crossref","first-page":"209","DOI":"10.1007\/s10653-006-9066-9","article-title":"Distribution and phytoavailability of antimony at an antimony mining and smelting area, Hunan, China","volume":"29","author":"M He","year":"2007","journal-title":"Environ Geochem Health"},{"key":"pone.0331138.ref014","doi-asserted-by":"crossref","first-page":"130252","DOI":"10.1016\/j.chemosphere.2021.130252","article-title":"Antimony, a pollutant of emerging concern: a review on industrial sources and remediation technologies","volume":"277","author":"PA Nishad","year":"2021","journal-title":"Chemosphere"},{"key":"pone.0331138.ref015","doi-asserted-by":"crossref","first-page":"102026","DOI":"10.1016\/j.eti.2021.102026","article-title":"A review of the environmental chemical behavior, detection and treatment of antimony","volume":"24","author":"Y Zhang","year":"2021","journal-title":"Environ Technol Innov"},{"issue":"10","key":"pone.0331138.ref016","doi-asserted-by":"crossref","first-page":"794","DOI":"10.3390\/w9100794","article-title":"The potential for the treatment of antimony-containing wastewater by iron-based adsorbents","volume":"9","author":"R-J Deng","year":"2017","journal-title":"Water"},{"key":"pone.0331138.ref017","doi-asserted-by":"crossref","first-page":"134047","DOI":"10.1016\/j.chemosphere.2022.134047","article-title":"Trivalent antimony removal using carbonaceous nanomaterial loaded with zero-valent bimetal (iron\/copper) and their effect on seed growth","volume":"296","author":"J Ji","year":"2022","journal-title":"Chemosphere"},{"key":"pone.0331138.ref018","doi-asserted-by":"crossref","first-page":"293","DOI":"10.1016\/S0011-9164(00)90027-4","article-title":"Effect of pH on the removal of arsenic and antimony using reverse osmosis membranes","volume":"131","author":"M Kang","year":"2000","journal-title":"Desalination"},{"key":"pone.0331138.ref019","first-page":"321","article-title":"Conceptual design for treatment of mining and metallurgical wastewaters which contains arsenic and antimony","volume":"18","author":"\u017d Kamberovi\u0107","year":"2012","journal-title":"Metall Mater Eng"},{"issue":"22","key":"pone.0331138.ref020","doi-asserted-by":"crossref","first-page":"3872","DOI":"10.3390\/w15223872","article-title":"Characterization of a moderately halotolerant antimony-removing desulfovibrio sp. strain isolated from landfill leachate","volume":"15","author":"CTK Pham","year":"2023","journal-title":"Water"},{"key":"pone.0331138.ref021","first-page":"4244","article-title":"Removal of antimony contaminant in water by electrocoagulation","volume":"8","author":"J Zhang","year":"2014","journal-title":"Chinese J Environ Eng"},{"issue":"33","key":"pone.0331138.ref022","doi-asserted-by":"crossref","first-page":"12911","DOI":"10.1021\/ie501727a","article-title":"Investigation of influencing factors and mechanism of antimony and arsenic removal by electrocoagulation using Fe\u2013Al electrodes","volume":"53","author":"P Song","year":"2014","journal-title":"Ind Eng Chem Res"},{"issue":"6","key":"pone.0331138.ref023","doi-asserted-by":"crossref","first-page":"483","DOI":"10.1023\/A:1024491019960","article-title":"Electrochemical reduction of As(III) and As(V) in acidic and basic solutions","volume":"33","author":"D Bejan","year":"2003","journal-title":"J Appl Electrochem"},{"issue":"4","key":"pone.0331138.ref024","first-page":"1338","article-title":"Removal of antimony in wastewater by electrochemical hydride generation and the recovery of antimony","volume":"36","author":"J Chen","year":"2015","journal-title":"Huan Jing Ke Xue"},{"issue":"4","key":"pone.0331138.ref025","doi-asserted-by":"crossref","first-page":"1288","DOI":"10.1039\/D2CS00570K","article-title":"Antimonene: a tuneable post-graphene material for advanced applications in optoelectronics, catalysis, energy and biomedicine","volume":"52","author":"JA Carrasco","year":"2023","journal-title":"Chem Soc Rev"},{"key":"pone.0331138.ref026","first-page":"655","article-title":"Environmental characteristics of water near the Xikuangshan antimony mine, Hunan Province","volume":"29","author":"J Zhu","year":"2009","journal-title":"Acta Scientiae Circumstantiae"},{"issue":"3","key":"pone.0331138.ref027","doi-asserted-by":"crossref","first-page":"598","DOI":"10.1016\/j.apgeochem.2011.12.005","article-title":"Arsenic and antimony contamination of waters, stream sediments and soils in the vicinity of abandoned antimony mines in the Western Carpathians, Slovakia","volume":"27","author":"E Hiller","year":"2012","journal-title":"Appl Geochem"},{"key":"pone.0331138.ref028","doi-asserted-by":"crossref","first-page":"148","DOI":"10.1016\/j.ibiod.2016.08.007","article-title":"Bioremoval of antimony from contaminated waters by a mixed batch culture of sulfate-reducing bacteria","volume":"115","author":"G Zhang","year":"2016","journal-title":"Inter Biodeterioration Biodegradation"},{"issue":"10","key":"pone.0331138.ref029","doi-asserted-by":"crossref","first-page":"2471","DOI":"10.1007\/s11368-016-1484-4","article-title":"Influence of reducing conditions on the release of antimony and arsenic from a tailings sediment","volume":"16","author":"Z Fu","year":"2016","journal-title":"J Soils Sediments"},{"issue":"6","key":"pone.0331138.ref030","doi-asserted-by":"crossref","first-page":"3029","DOI":"10.1039\/C4TA03893B","article-title":"Sustainable production of formic acid by electrolytic reduction of gaseous carbon dioxide","volume":"3","author":"S Lee","year":"2015","journal-title":"J Mater Chem A"},{"issue":"11","key":"pone.0331138.ref031","doi-asserted-by":"crossref","DOI":"10.1149\/2.0221611jes","article-title":"Hydrogen permeation in PEM electrolyzer cells operated at asymmetric pressure conditions","volume":"163","author":"P Trinke","year":"2016","journal-title":"J Electrochem Soc"},{"issue":"25","key":"pone.0331138.ref032","doi-asserted-by":"crossref","first-page":"7787","DOI":"10.1021\/jacs.8b04006","article-title":"Explanation of dramatic ph-dependence of hydrogen binding on noble metal electrode: greatly weakened water adsorption at high pH","volume":"140","author":"T Cheng","year":"2018","journal-title":"J Am Chem Soc"},{"issue":"2","key":"pone.0331138.ref033","doi-asserted-by":"crossref","DOI":"10.1149\/2.0881802jes","article-title":"Perspective\u2014towards establishing apparent hydrogen binding energy as the descriptor for hydrogen oxidation\/evolution reactions","volume":"165","author":"J Zheng","year":"2018","journal-title":"J Electrochem Soc"},{"issue":"2","key":"pone.0331138.ref034","article-title":"Review and prospects of PEM water electrolysis at elevated temperature operation","volume":"9","author":"M Bonanno","year":"2023","journal-title":"Adv Materials Technol"},{"key":"pone.0331138.ref035","doi-asserted-by":"crossref","first-page":"138046","DOI":"10.1016\/j.electacta.2021.138046","article-title":"Insight into elevated temperature and thin membrane application for high efficiency in polymer electrolyte water electrolysis","volume":"377","author":"S Garbe","year":"2021","journal-title":"Electrochimica Acta"},{"issue":"10","key":"pone.0331138.ref036","doi-asserted-by":"crossref","first-page":"1084","DOI":"10.1021\/j150532a024","article-title":"The thermal decomposition of stibine","volume":"59","author":"K Tamaru","year":"1955","journal-title":"J Phys Chem"},{"key":"pone.0331138.ref037","first-page":"673","article-title":"The temperature effect of reacting solution on the hydride generation and the stability of hydride","author":"B Gong","year":"1985","journal-title":"Chinese J Anal Chem"},{"key":"pone.0331138.ref038","doi-asserted-by":"crossref","first-page":"115371","DOI":"10.1016\/j.jelechem.2021.115371","article-title":"Surface sulfuration of antimony oxide enhances the electrochemical determination of acebutolol in biomedical samples","volume":"894","author":"AS Haidyrah","year":"2021","journal-title":"J Electroanal Chem"},{"issue":"4","key":"pone.0331138.ref039","doi-asserted-by":"crossref","first-page":"1068","DOI":"10.3390\/w12041068","article-title":"Use of ultrasound as an advanced oxidation process for the degradation of emerging pollutants in water","volume":"12","author":"AL Camargo-Perea","year":"2020","journal-title":"Water"},{"issue":"3","key":"pone.0331138.ref040","doi-asserted-by":"crossref","first-page":"259","DOI":"10.1007\/s10311-016-0568-0","article-title":"Degradation of pharmaceuticals by ultrasound-based advanced oxidation process","volume":"14","author":"MP Rayaroth","year":"2016","journal-title":"Environ Chem Lett"},{"key":"pone.0331138.ref041","doi-asserted-by":"crossref","first-page":"13801","DOI":"10.1038\/srep13801","article-title":"Insight on Tafel slopes from a microkinetic analysis of aqueous electrocatalysis for energy conversion","volume":"5","author":"T Shinagawa","year":"2015","journal-title":"Sci Rep"},{"issue":"29","key":"pone.0331138.ref042","doi-asserted-by":"crossref","first-page":"8184","DOI":"10.1021\/acs.langmuir.5b01825","article-title":"Dynamics of single hydrogen bubbles at a platinum microelectrode","volume":"31","author":"X Yang","year":"2015","journal-title":"Langmuir"},{"issue":"1","key":"pone.0331138.ref043","doi-asserted-by":"crossref","first-page":"23","DOI":"10.1007\/s11837-018-3191-7","article-title":"CFD simulations of gas\u2013liquid multiscale flow characteristics in an aluminum electrolysis cell with population balance model: effect of anode slot configuration","volume":"71","author":"S Zhan","year":"2018","journal-title":"JOM"}],"container-title":["PLOS One"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/dx.plos.org\/10.1371\/journal.pone.0331138","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2025,9,4]],"date-time":"2025-09-04T17:30:14Z","timestamp":1757007014000},"score":1,"resource":{"primary":{"URL":"https:\/\/dx.plos.org\/10.1371\/journal.pone.0331138"}},"subtitle":[],"editor":[{"given":"Hailing","family":"Ma","sequence":"first","affiliation":[],"role":[{"role":"editor","vocabulary":"crossref"}]}],"short-title":[],"issued":{"date-parts":[[2025,9,4]]},"references-count":43,"journal-issue":{"issue":"9","published-online":{"date-parts":[[2025,9,4]]}},"URL":"https:\/\/doi.org\/10.1371\/journal.pone.0331138","relation":{},"ISSN":["1932-6203"],"issn-type":[{"type":"electronic","value":"1932-6203"}],"subject":[],"published":{"date-parts":[[2025,9,4]]}}}