ACS ES&T engineeringPub Date : 2025-03-20DOI: 10.1021/acsestengg.4c0094310.1021/acsestengg.4c00943
Ke-Lin Yu, Xiaojun Wang, Chunying Wang, Shaohua Chen, Sheng-Peng Sun*, John C. Crittenden and Yao-Yin Lou*,
{"title":"Dynamic Control of Atomic Hydrogen for Electrochemical Nitrate Reduction Coupled with Anammox Autotrophic Nitrogen Removal","authors":"Ke-Lin Yu, Xiaojun Wang, Chunying Wang, Shaohua Chen, Sheng-Peng Sun*, John C. Crittenden and Yao-Yin Lou*, ","doi":"10.1021/acsestengg.4c0094310.1021/acsestengg.4c00943","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00943https://doi.org/10.1021/acsestengg.4c00943","url":null,"abstract":"<p >Anaerobic ammonium oxidation (anammox) is the most cost-effective and low-carbon biological nitrogen removal technology and is very sensitive to the ammonia/nitrite ratio. Bioinspired by the dissimilatory nitrate reduction process, for the first time, we built an electric field-driven dissimilatory nitrate reduction (eDNR) process coupled with anammox (eDNR-anammox) to achieve low-carbon and efficient nitrogen removal from nitrate-rich industrial wastewater. The eDNR process, utilizing a copper nanowire catalyst with abundant oxygen vacancies as a model catalyst, enables the potential-dependent provision of atomic hydrogen that facilitates nitrate reduction into tunable ratios of nitrite and ammonium. This tunability supports successful conversion of the formed nitrogen species into dinitrogen by the anammox process, with over 90% total nitrogen removal. Compared to the partial-denitrification-anammox process, the eDNR-anammox process reduces organic requirements by 100%, sludge production by 70%, and nitrous oxide emissions by 2 orders of magnitude.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 6","pages":"1441–1450 1441–1450"},"PeriodicalIF":7.4,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144269892","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS ES&T engineeringPub Date : 2025-03-18DOI: 10.1021/acsestengg.4c0094910.1021/acsestengg.4c00949
Lu Chen, Guanqing Song, Xiao Wang*, Chi Song, Haijiao Xie, Jing Sun*, Fan Dong and Deliang Chen*,
{"title":"Regulation on the Exposure Degree and Lewis Acidity of Fe–O Sites in Fe-MOGs for Photocatalytic Oxidation of o-Xylene","authors":"Lu Chen, Guanqing Song, Xiao Wang*, Chi Song, Haijiao Xie, Jing Sun*, Fan Dong and Deliang Chen*, ","doi":"10.1021/acsestengg.4c0094910.1021/acsestengg.4c00949","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00949https://doi.org/10.1021/acsestengg.4c00949","url":null,"abstract":"<p >Adsorption and catalytic sites in photocatalysts are important factors influencing the degradation efficiency of aromatic volatile organic compounds (VOCs), and their accurate regulation is the prerequisite to reveal the photocatalytic oxidation (PCO) mechanisms. Herein, by adjusting the molar ratio between Fe salts and H<sub>3</sub>BTC linkers, the coordinate saturation degree and Lewis acidity of open Fe–O sites in Fe-MOGs were successfully modulated, which follows the order of Fe<sub>1</sub>BTC<sub>0.5</sub> > Fe<sub>1</sub>BTC<sub>1</sub> > Fe<sub>1</sub>BTC<sub>2</sub>. The highly exposed Fe–O sites (Fe<sub>1</sub>BTC<sub>0.5</sub>) not only promote the adsorption of <i>o</i>-xylene via Lewis acid–base and π–π interactions but also accelerate the generation of oxidative ·OH and ·O<sub>2</sub><sup>–</sup> radicals by providing active open metal sites (OMSs). However, highly exposed Fe–O sites inhibit the release of benzyl midproducts, which detriments the performance of Fe<sub>1</sub>BTC<sub>0.5</sub>. Fe<sub>1</sub>BTC<sub>1</sub> with an appropriate exposure degree of Fe–O sites and excellent photoelectric properties shows moderate affinity to <i>o</i>-xylene and sufficient oxidative radicals, which enable the efficient and stable removal of <i>o</i>-xylene (80% for at least 180 min). <i>In situ</i> diffuse reflection infrared Fourier transform (DRIFT) spectra reveal the impacts of exposure degree of Fe–O sites on the PCO pathway of <i>o</i>-xylene. Our study provides novel insights into the role of adsorption and catalytic sites in the elimination of aromatic VOCs.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 6","pages":"1477–1489 1477–1489"},"PeriodicalIF":7.4,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144269891","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS ES&T engineeringPub Date : 2025-03-17DOI: 10.1021/acsestengg.4c0096310.1021/acsestengg.4c00963
Shuaiyi Shi, Lin Chen, Yufei Zhang, Jingyuan Cui*, Shuran Zhang, Chenliu Tang* and Xiang Hu,
{"title":"Sulfidated Nanoscale Zero-Valent Iron (S-nZVI) Facilitates Remediation and Safe Crop Production in Cr(VI) and Microplastics Co-contaminated Soil","authors":"Shuaiyi Shi, Lin Chen, Yufei Zhang, Jingyuan Cui*, Shuran Zhang, Chenliu Tang* and Xiang Hu, ","doi":"10.1021/acsestengg.4c0096310.1021/acsestengg.4c00963","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00963https://doi.org/10.1021/acsestengg.4c00963","url":null,"abstract":"<p >Emerging Cr(VI)-microplastics (MPs) co-contamination in agricultural soil poses an increasing environmental and food safety risk, primarily due to their joint toxic effects on the soil–plant system (e.g., the “Trojan horse” effect). To address this issue, sulfidated nanoscale zerovalent iron (S-nZVI) is utilized as a remediation agent. S-nZVI possesses a metallic iron core that rapidly reduces Cr(VI) to Cr(III), while the surface layer contains high-density sites for attracting and absorbing MPs, resulting in larger aggregates and lowering their mobility and solubility in soil. Results show that the application of S-nZVI at 0.5 wt % achieves a Cr(VI) removal efficiency of over 98.74% for total Cr(VI) concentrations, as well as facilitates the transformation of 40% of Cr into the favorable Oxidizable and Residual fractions. Exemplified by lettuce planting, the pot experiment proves the greater toxicity of Cr(VI)-MPs co-contamination than individual contaminations, evidenced by the decreased plant biomass and elevated ROS levels. Conversely, lettuce grown in remediated soil keeps a well-developed growth, with Cr levels of 0.03–0.05 mg/g dry weight, and MPs not entering the body, reaching safe levels. In contaminated soils worldwide, these findings provide new insights into the application of nanoscale zerovalent iron technology for remediation and crop safety.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 6","pages":"1513–1524 1513–1524"},"PeriodicalIF":7.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144269890","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS ES&T engineeringPub Date : 2025-03-17DOI: 10.1021/acsestengg.4c0057610.1021/acsestengg.4c00576
Le Fang, Guangcai Tan, Weiwei Xuan, Jiaming Liang, Liping Li, Shaogang Hu*, Zhenshan Li* and Siqi Tang*,
{"title":"Heat Capacity-Manipulated Balance in Phosphorus Bioavailability Enhancement and Heavy Metal Stabilization during Sewage Sludge Copyrolysis","authors":"Le Fang, Guangcai Tan, Weiwei Xuan, Jiaming Liang, Liping Li, Shaogang Hu*, Zhenshan Li* and Siqi Tang*, ","doi":"10.1021/acsestengg.4c0057610.1021/acsestengg.4c00576","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00576https://doi.org/10.1021/acsestengg.4c00576","url":null,"abstract":"<p >Disentangling the thermochemistry of sludge copyrolysis to balance phosphorus (P) bioavailability enhancement and heavy metal (HM) stabilization is challenging due to intricate and disordering thermochemical reactions caused by sludge compositional inhomogeneity. A heat capacity assembly and dispatch strategy via antagonistic additive-paired sludge copyrolysis was conceived to quantitatively determine the balance for P reclamation from sewage sludge (SS). Calcium oxide (CaO, with additions ranging from 7.54 to 10%) and wasted rapeseed meal (RM, with additions ranging from 10 to 50%)-formulated copyrolysis experiments were designed to investigate the evolved fate of P and HMs in SS-derived biochar (SSB) production. Ryegrass plant cultivation was adopted to examine the orchestrated balance of P and HMs in soil applications. RM and CaO preferentially influenced the P distribution, including iron/aluminum-bound P and apatite/CaCO<sub>3</sub>-associated P, respectively. In contrast, both additives consistently reached equilibrium with two HM ensembles, including soluble/reducible and oxidizable/residual fractions. SSB derived from RM-added (50% addition) and CaO-RM-paired (6% CaO and 47% RM addition) copyrolysis at 700 °C demonstrated preferential P acquisition of ryegrass (height increase by 17.4 and 4%, respectively) while maintaining a low HM ecological risk index (27.5 and 16.3, respectively). The kinetic and thermodynamic results confirmed that CaO and RM had antagonistic effects on the thermochemistry of sludge copyrolysis. The heat capacity reached its maximum at around 675 °C and was not affected by the paired additives. The outcome can rationalize P upcycling from SS-like waste resources through tapping the heat capacity precisely tuning the thermochemistry of copyrolysis, thereby boosting global P circularity.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 4","pages":"839–854 839–854"},"PeriodicalIF":7.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143818916","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS ES&T engineeringPub Date : 2025-03-15DOI: 10.1021/acsestengg.4c0095110.1021/acsestengg.4c00951
Yaqiong Luo, Jiacheng Bao, Xin Yan, Lei Shi, Fei Wang, Xin Sun*, Kai Li* and Ping Ning,
{"title":"Wet de-NOx Process of the Composite Phosphate Rock/H2O2 Slurry by Calcination Modification: Key Components and Radical Generation","authors":"Yaqiong Luo, Jiacheng Bao, Xin Yan, Lei Shi, Fei Wang, Xin Sun*, Kai Li* and Ping Ning, ","doi":"10.1021/acsestengg.4c0095110.1021/acsestengg.4c00951","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00951https://doi.org/10.1021/acsestengg.4c00951","url":null,"abstract":"<p >Wet flue gas denitrification offers a new route for converting industrial nitrogen oxides (NOx) into highly concentrated nitrate wastewater. This study presents a novel H<sub>2</sub>O<sub>2</sub>-based advanced oxidation process that utilizes the composite calcined phosphate rock to activate H<sub>2</sub>O<sub>2</sub> for efficient NOx removal. The calcination treatment for composite phosphate rocks was found to enhance de-NOx efficiency and capacity by varying the CaMg(CO<sub>3</sub>)<sub>2</sub> and Ca<sub>5</sub>(PO<sub>4</sub>)<sub>3</sub>OH contents and creating oxygen vacancies. A systematic investigation of the phase structural evolution under alkaline H<sub>2</sub>O<sub>2</sub> conditions identified CaMg(CO<sub>3</sub>)<sub>2</sub> and Ca<sub>5</sub>(PO<sub>4</sub>)<sub>3</sub>OH as the primary active components, with CaMg(CO<sub>3</sub>)<sub>2</sub> preferentially participating in the reaction. Radical quenching experiments and time-resolved electron paramagnetic resonance (EPR) analysis confirmed the predominant roles of superoxide radicals (O<sub>2</sub><sup>•–</sup>) and surface-bound hydroxyl radicals (<sup>•</sup>OH<sub>surface</sub>) in NOx oxidation. A mechanistic pathway was proposed, highlighting the synergistic effects of reactive oxygen species (ROS) and mineral phase transitions on NOx removal. The proposed NOx purification method offers a promising option for nitrogen recovery and NOx pollution control.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 6","pages":"1490–1501 1490–1501"},"PeriodicalIF":7.4,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144269879","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Rose S. Kantor*, Lauren C. Kennedy, Scott E. Miller, Jorien Favere and Kara L. Nelson*,
{"title":"","authors":"Rose S. Kantor*, Lauren C. Kennedy, Scott E. Miller, Jorien Favere and Kara L. Nelson*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 3","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":7.4,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsestengg.4c00665","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144434548","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}