With the continuous development of new energy technologies, there is a growing need for highly efficient, economical, and robust trifunctional electrocatalysts for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) to meet the demanding requirements of applications, such as rechargeable zinc-air batteries (ZABs) and overall water splitting, particularly under high current conditions. Unfortunately, most current research on trifunctional catalysts is limited to water electrolysis at low current densities, which restricts their practical application. To address this issue, in this work, through an integrated multistage structural design combined with a cerium oxide coating, we have developed a trifunctional catalyst capable of efficient overall water splitting at high current densities, with enhanced stability. The CoFe@CNT@CeO2/IF (Iron foam) catalyst exhibits a half-wave potential of 0.822 V for ORR. At a high current density of 500 mA·cm–2, it shows an HER overpotential of 314 mV, with stable electrochemical performance maintained for 90 h. The OER overpotential is 403 mV, with stable electrochemical performance sustained for 96 h. In addition, the assembled ZAB demonstrates a power density of 135.75 mW·cm–2, and self-driven overall water splitting is successfully realized using this catalyst. These results demonstrate that the prepared trifunctional catalyst holds significant promise for energy storage and conversion applications.
{"title":"An Efficient Trifunctional Electrocatalyst for High-Current-Density Overall Water Splitting Self-Driven by Zinc–Air Batteries: Synergistic Enhancement through Hierarchical Structure Design and Cerium Oxide Coating","authors":"Qihong Zhou, Jiajun Lai, Jinming Zeng, Chao Liu, Huan Li, Xiaoping Zou, Xiaopeng Qi, Tongxiang Liang","doi":"10.1021/acssuschemeng.5c12250","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c12250","url":null,"abstract":"With the continuous development of new energy technologies, there is a growing need for highly efficient, economical, and robust trifunctional electrocatalysts for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) to meet the demanding requirements of applications, such as rechargeable zinc-air batteries (ZABs) and overall water splitting, particularly under high current conditions. Unfortunately, most current research on trifunctional catalysts is limited to water electrolysis at low current densities, which restricts their practical application. To address this issue, in this work, through an integrated multistage structural design combined with a cerium oxide coating, we have developed a trifunctional catalyst capable of efficient overall water splitting at high current densities, with enhanced stability. The CoFe@CNT@CeO<sub>2</sub>/IF (Iron foam) catalyst exhibits a half-wave potential of 0.822 V for ORR. At a high current density of 500 mA·cm<sup>–2</sup>, it shows an HER overpotential of 314 mV, with stable electrochemical performance maintained for 90 h. The OER overpotential is 403 mV, with stable electrochemical performance sustained for 96 h. In addition, the assembled ZAB demonstrates a power density of 135.75 mW·cm<sup>–2</sup>, and self-driven overall water splitting is successfully realized using this catalyst. These results demonstrate that the prepared trifunctional catalyst holds significant promise for energy storage and conversion applications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"19 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147358881","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-05DOI: 10.1021/acssuschemeng.5c13785
Zhipeng Gan, Chunming Ye, Xinan Chen, Zizhong Zhang, Tao Ji, Wenyue Su
Rationally loading a highly dispersed cocatalyst onto a photocatalyst greatly enhances photocatalytic performance. In this study, Ni-MOF-74 acts as a slow-release source of Ni2+ to synthesize NiS/Cd0.7Zn0.3S (NiS/CZS) via a one-pot method. The gradual release of trace Ni2+ ensures the uniform dispersion and deposition of NiS on CZS. Compared with Ni(NO3)2-derived NiS-CZS and pure CZS, the NiS/CZS composite exhibits markedly improved performance in visible-light-driven benzyl alcohol (BA) oxidation coupled with hydrogen evolution. After 3 h of irradiation, the optimized 12% NiS/CZS achieves 69.5% BA conversion, 18.2 times that of the Ni(NO3)2-derived sample and 31 times that of pure CZS. This improvement arises from the uniform NiS deposition, which enhances the interaction between NiS and CZS, increases interfacial contact, shortens the electron migration distance, and suppresses charge recombination. In situ DRIFTS and EPR analyses unveil the complete pathway of intermediate formation and transformation. This work presents a controllable strategy for uniform cocatalyst deposition, offering an effective approach to boost photocatalytic efficiency.
{"title":"Ni-MOF-74-Derived NiS/Cd0.7Zn0.3S Boosts Photocatalytic Benzyl Alcohol Oxidation Coupled with H2 Evolution","authors":"Zhipeng Gan, Chunming Ye, Xinan Chen, Zizhong Zhang, Tao Ji, Wenyue Su","doi":"10.1021/acssuschemeng.5c13785","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c13785","url":null,"abstract":"Rationally loading a highly dispersed cocatalyst onto a photocatalyst greatly enhances photocatalytic performance. In this study, Ni-MOF-74 acts as a slow-release source of Ni<sup>2+</sup> to synthesize NiS/Cd<sub>0.7</sub>Zn<sub>0.3</sub>S (NiS/CZS) via a one-pot method. The gradual release of trace Ni<sup>2+</sup> ensures the uniform dispersion and deposition of NiS on CZS. Compared with Ni(NO<sub>3</sub>)<sub>2</sub>-derived NiS-CZS and pure CZS, the NiS/CZS composite exhibits markedly improved performance in visible-light-driven benzyl alcohol (BA) oxidation coupled with hydrogen evolution. After 3 h of irradiation, the optimized 12% NiS/CZS achieves 69.5% BA conversion, 18.2 times that of the Ni(NO<sub>3</sub>)<sub>2</sub>-derived sample and 31 times that of pure CZS. This improvement arises from the uniform NiS deposition, which enhances the interaction between NiS and CZS, increases interfacial contact, shortens the electron migration distance, and suppresses charge recombination. In situ DRIFTS and EPR analyses unveil the complete pathway of intermediate formation and transformation. This work presents a controllable strategy for uniform cocatalyst deposition, offering an effective approach to boost photocatalytic efficiency.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"31 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147358816","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-04DOI: 10.1021/acssuschemeng.5c13803
Karthick Raj Selvam,Tizazu H Mekonnen
Silk fibroin nanofibers are promising biomaterials for tissue engineering, wound healing, and controlled release, owing to their biocompatibility, biodegradability, and mechanical robustness. This study demonstrates a scalable route for producing regenerated silk fibroin (RSF) nanofibers using solution blow spinning (SBS) and establishes how degumming, doping rheology, and cellulose nanocrystal (CNC) reinforcement collectively govern fiber formation and performance. Three degumming methods, boiling water, autoclave treatment, and sodium carbonate, were systematically compared, revealing significant differences in sericin removal efficiency, viscosity-average molecular weight, and secondary structure. RSF was regenerated through lithium bromide dissolution and ethanol-induced phase separation, eliminating the need for dialysis. A 10 wt % RSF dope provided optimal rheological behavior for SBS, while CNC incorporation (0.5–1.5 wt %) increased viscosity moderately and promoted finer jet stretching. Furthermore, CNC addition enhanced molecular ordering, increased the β-sheet content and crystallinity, reduced the fiber diameter, and significantly improved tensile properties. Uniform, bead-free nanofiber mats were obtained, and characterization by scanning electron microscopy, Fourier transform infrared spectroscopy, wide angle X-ray diffraction (WAXD), thermogravimetric analysis, and mechanical testing confirmed CNC-induced structural refinement and reinforcement. Overall, this work establishes SBS as a practical platform for producing structurally tunable RSF/CNC nanofibers and identifies key processing–structure–property relationships relevant to biomedical applications, including future integration of bioactive agents for sustained release.
{"title":"Solution Blow Spinning and Molecular Ordering of Regenerated Silk Fibroin: Linking Degumming, Rheology, and CNC-Induced β-Sheet Formation","authors":"Karthick Raj Selvam,Tizazu H Mekonnen","doi":"10.1021/acssuschemeng.5c13803","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c13803","url":null,"abstract":"Silk fibroin nanofibers are promising biomaterials for tissue engineering, wound healing, and controlled release, owing to their biocompatibility, biodegradability, and mechanical robustness. This study demonstrates a scalable route for producing regenerated silk fibroin (RSF) nanofibers using solution blow spinning (SBS) and establishes how degumming, doping rheology, and cellulose nanocrystal (CNC) reinforcement collectively govern fiber formation and performance. Three degumming methods, boiling water, autoclave treatment, and sodium carbonate, were systematically compared, revealing significant differences in sericin removal efficiency, viscosity-average molecular weight, and secondary structure. RSF was regenerated through lithium bromide dissolution and ethanol-induced phase separation, eliminating the need for dialysis. A 10 wt % RSF dope provided optimal rheological behavior for SBS, while CNC incorporation (0.5–1.5 wt %) increased viscosity moderately and promoted finer jet stretching. Furthermore, CNC addition enhanced molecular ordering, increased the β-sheet content and crystallinity, reduced the fiber diameter, and significantly improved tensile properties. Uniform, bead-free nanofiber mats were obtained, and characterization by scanning electron microscopy, Fourier transform infrared spectroscopy, wide angle X-ray diffraction (WAXD), thermogravimetric analysis, and mechanical testing confirmed CNC-induced structural refinement and reinforcement. Overall, this work establishes SBS as a practical platform for producing structurally tunable RSF/CNC nanofibers and identifies key processing–structure–property relationships relevant to biomedical applications, including future integration of bioactive agents for sustained release.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"12 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147346666","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Coal-based needle coke can be converted into artificial graphite via high-temperature graphitization to serve as the anode material in the preparation of silicon/graphite composites. However, the graphitization treatment is an energy-intensive process, and the rigid structure of graphite imposes a limitation on the silicon content in silicon/graphite composites. To address these challenges, this study employed a nickel-catalyzed low-temperature graphitization strategy. This method generated multilayer hollow graphene spheres on the graphitized needle coke, forming a distinct architecture that effectively buffers silicon volume expansion and ensures the structural stability. With the further enhancement of overall electrical conductivity provided by a few-layer graphene coating, the silicon/graphite composite electrode prepared with a nickel acetate to needle coke mass ratio of 8:1 delivered the optimal electrochemical performance, achieving a highly reversible specific capacity of 983.4 mAh g–1 at a current density of 0.2 A g–1 and a high capacity retention of 92.0% after 1000 cycles at 1 A g–1. Moreover, as a practical application, the full cell delivers an outstanding capacity retention of 89.7% after 100 cycles at 1C, demonstrating considerable promise for commercial application.
煤基针状焦炭经高温石墨化可转化为人造石墨，作为制备硅/石墨复合材料的负极材料。然而，石墨化处理是一个能源密集型的过程，石墨的刚性结构限制了硅/石墨复合材料中硅的含量。为了解决这些挑战，本研究采用了镍催化的低温石墨化策略。该方法在石墨化针状焦炭上生成多层空心石墨烯球，形成独特的结构，有效缓冲硅体积膨胀，保证结构稳定性。随着少层石墨烯涂层进一步提高整体电导率，以醋酸镍与针状焦炭质量比为8:1制备的硅/石墨复合电极具有最佳的电化学性能，在0.2 a g-1电流密度下达到983.4 mAh g-1的高可逆比容量，在1 a g-1电流密度下1000次循环后容量保持率高达92.0%。此外，作为实际应用，在1C下进行100次循环后，全电池的容量保持率为89.7%，显示出相当大的商业应用前景。
{"title":"Constructing Multilayer Hollow Graphene Spheres on Needle Coke Via Nickel Acetate Catalysis for High-Performance Silicon/Graphite Composite Anodes","authors":"Yujun Li,Yonggang Wang,Xinli Liu,Delin Wang,Haiyong Zhang","doi":"10.1021/acssuschemeng.5c11978","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c11978","url":null,"abstract":"Coal-based needle coke can be converted into artificial graphite via high-temperature graphitization to serve as the anode material in the preparation of silicon/graphite composites. However, the graphitization treatment is an energy-intensive process, and the rigid structure of graphite imposes a limitation on the silicon content in silicon/graphite composites. To address these challenges, this study employed a nickel-catalyzed low-temperature graphitization strategy. This method generated multilayer hollow graphene spheres on the graphitized needle coke, forming a distinct architecture that effectively buffers silicon volume expansion and ensures the structural stability. With the further enhancement of overall electrical conductivity provided by a few-layer graphene coating, the silicon/graphite composite electrode prepared with a nickel acetate to needle coke mass ratio of 8:1 delivered the optimal electrochemical performance, achieving a highly reversible specific capacity of 983.4 mAh g–1 at a current density of 0.2 A g–1 and a high capacity retention of 92.0% after 1000 cycles at 1 A g–1. Moreover, as a practical application, the full cell delivers an outstanding capacity retention of 89.7% after 100 cycles at 1C, demonstrating considerable promise for commercial application.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"129 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147346686","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-04DOI: 10.1021/acssuschemeng.6c00851
Xiaowen Zhang,Yuanyuan You,Yansong Yang,Jiahuan Li,Fangfang Zhao,Kuiyi You,He’an Luo
The industrial application of traditional tertiary amine solutions for CO2 absorption is limited by their slow absorption rates. Therefore, this study aims to synthesize mesoporous MgO nanoparticles through a simple method and utilize them to catalytically speed up the absorption of CO2 in representative tertiary amine MDEA solutions. This study primarily employed five magnesium sources as precursors to produce MgO nanoparticles through calcination. Among these, the MgO derived from the Mg(OH)2 precursor exhibited the most effective catalytic performance for CO2 absorption in MDEA solutions. Compared to the noncatalytic test, MgO-MgH achieved a 302.2% increase in the CO2 absorption rate and an 82.6% increase in absorption capacity. The superior CO2 absorption efficiency of the MgO-MgH catalyst is mainly attributed to its abundant surface alkaline sites and oxygen vacancies. Online FT-IR characterization results evidenced the catalytic role of MgO-MgH in facilitating the CO2 absorption process. A possible catalytic absorption mechanism over MgO-MgH is proposed. Moreover, the MgO-MgH’s stability was confirmed through a ten-cycle CO2 absorption–desorption study. This study proposes a method to enhance CO2 absorption by incorporating an easily synthesized alkaline nanomaterial, MgO-MgH, effectively overcoming its drawback and advancing the practical application of tertiary amine absorbents for CO2 capture.
{"title":"Facile Synthesis of Highly Efficient MgO for Catalytically Accelerating CO2 Absorption in Tertiary Amine Solutions","authors":"Xiaowen Zhang,Yuanyuan You,Yansong Yang,Jiahuan Li,Fangfang Zhao,Kuiyi You,He’an Luo","doi":"10.1021/acssuschemeng.6c00851","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c00851","url":null,"abstract":"The industrial application of traditional tertiary amine solutions for CO2 absorption is limited by their slow absorption rates. Therefore, this study aims to synthesize mesoporous MgO nanoparticles through a simple method and utilize them to catalytically speed up the absorption of CO2 in representative tertiary amine MDEA solutions. This study primarily employed five magnesium sources as precursors to produce MgO nanoparticles through calcination. Among these, the MgO derived from the Mg(OH)2 precursor exhibited the most effective catalytic performance for CO2 absorption in MDEA solutions. Compared to the noncatalytic test, MgO-MgH achieved a 302.2% increase in the CO2 absorption rate and an 82.6% increase in absorption capacity. The superior CO2 absorption efficiency of the MgO-MgH catalyst is mainly attributed to its abundant surface alkaline sites and oxygen vacancies. Online FT-IR characterization results evidenced the catalytic role of MgO-MgH in facilitating the CO2 absorption process. A possible catalytic absorption mechanism over MgO-MgH is proposed. Moreover, the MgO-MgH’s stability was confirmed through a ten-cycle CO2 absorption–desorption study. This study proposes a method to enhance CO2 absorption by incorporating an easily synthesized alkaline nanomaterial, MgO-MgH, effectively overcoming its drawback and advancing the practical application of tertiary amine absorbents for CO2 capture.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"15 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147346661","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-04DOI: 10.1021/acssuschemeng.5c13620
Yuanwei Ma,Lanyan Li,Qiang Liu,Wenling Yang,Xinyu Cao,Yujia He,Jigang Wang,Zhongfang Li,Likai Wang
The advancement of metal-air batteries critically depends on the rational design of cost-effective, highly active, and durable bifunctional oxygen electrocatalysts. Herein, we present a facile strategy to synthesize monodisperse PtCo nanoparticles (NPs) confined within N, P, and S codoped porous carbon (PtCo-NPSC), leveraging multiheteroatom doping and nanoconfinement to precisely modulate the catalyst’s interfacial electronic structure. The nitrogen-doped carbon shell prevents aggregation, while the strong coupling between PtCo NPs and the heteroatom-rich carbon framework optimizes the electronic states of active sites, synergistically enhancing the oxygen reduction reaction/OER activity. When applied as a cathode catalyst, PtCo-NPSC enables rechargeable zinc-air batteries (ZABs) to achieve an outstanding power density of 220 mW cm–2 and a specific capacity of 779.4 mAh g–1Zn. The corresponding solid-state ZAB also demonstrates superior performance with a peak power density of 102 mW cm–2 and a prolonged cycle life of 230 h. This work highlights a generalizable design paradigm-integrating NP confinement with multiheteroatom carbon engineering to achieve high-performance, durable electrocatalysts for next-generation energy storage applications.
金属-空气电池的发展关键取决于合理设计高性价比、高活性和耐用的双功能氧电催化剂。在此，我们提出了一种简单的策略来合成限制在N， P和S共掺杂多孔碳（PtCo- npsc）内的单分散PtCo纳米颗粒（NPs），利用多杂原子掺杂和纳米限制来精确调节催化剂的界面电子结构。氮掺杂的碳壳防止了聚集，而PtCo NPs与富杂原子碳框架之间的强耦合优化了活性位点的电子态，协同提高了氧还原反应/OER活性。当用作阴极催化剂时，PtCo-NPSC使可充电锌空气电池（ZABs）实现220 mW cm-2的卓越功率密度和779.4 mAh g-1Zn的比容量。相应的固态ZAB也表现出优异的性能，峰值功率密度为102 mW cm-2，循环寿命延长至230小时。这项工作强调了一种可推广的设计范例——将NP约束与多杂原子碳工程相结合，以实现高性能、耐用的电催化剂，用于下一代储能应用。
{"title":"PtCo Nanoparticles Confined in N, P, and S Codoped Porous Carbon for Ultralong Solid-State Zn-Air Batteries","authors":"Yuanwei Ma,Lanyan Li,Qiang Liu,Wenling Yang,Xinyu Cao,Yujia He,Jigang Wang,Zhongfang Li,Likai Wang","doi":"10.1021/acssuschemeng.5c13620","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c13620","url":null,"abstract":"The advancement of metal-air batteries critically depends on the rational design of cost-effective, highly active, and durable bifunctional oxygen electrocatalysts. Herein, we present a facile strategy to synthesize monodisperse PtCo nanoparticles (NPs) confined within N, P, and S codoped porous carbon (PtCo-NPSC), leveraging multiheteroatom doping and nanoconfinement to precisely modulate the catalyst’s interfacial electronic structure. The nitrogen-doped carbon shell prevents aggregation, while the strong coupling between PtCo NPs and the heteroatom-rich carbon framework optimizes the electronic states of active sites, synergistically enhancing the oxygen reduction reaction/OER activity. When applied as a cathode catalyst, PtCo-NPSC enables rechargeable zinc-air batteries (ZABs) to achieve an outstanding power density of 220 mW cm–2 and a specific capacity of 779.4 mAh g–1Zn. The corresponding solid-state ZAB also demonstrates superior performance with a peak power density of 102 mW cm–2 and a prolonged cycle life of 230 h. This work highlights a generalizable design paradigm-integrating NP confinement with multiheteroatom carbon engineering to achieve high-performance, durable electrocatalysts for next-generation energy storage applications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"100 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147346664","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-04DOI: 10.1021/acssuschemeng.5c11743
Xiaoyun Du,Zhiyuan Shao,Jun Chang,Kai Cui
Limestone calcined clay cement (LC3) is widely recognized as a sustainable cementitious material. However, the low reactivity of natural limestone often limits the early carbon aluminate reaction and compromises the early compressive strength of LC3. This study proposes the preparation of highly active CaCO3 by carbonating SS, RCP, MS, and CS. The resulting product is then used to replace limestone and activate early carbon aluminate reactions in LC3. This strategy aims to develop a sustainable engineering material with high compressive strength and low CO2 emissions, referred to as carbonated waste calcined clay cement (CWC3). The results showed that compared with LC3, the compressive strength of CWC3 at 3 and 28 days increased by 19.7% and 10.8%, respectively, while the CO2 emissions and CO2 index decreased by 14.4% and 21.9%, respectively. The mechanism of early activation of the CWC3 carbon aluminate reaction includes two aspects: the crystallite grain size and crystallinity of CaCO3 in carbonated waste are much smaller and lower than those of CaCO3 in natural limestone with a polycrystalline crystal cluster morphology. This structure introduces a higher density of crystal defects, thereby enhancing chemical reactivity. CaCO3 crystal clusters and silica gel are interlaced in a carbonated waste particle, and the volcanic ash reaction of silica gel disperses the CaCO3 crystal clusters, thereby inducing more carbon aluminate reaction interfaces. In addition, the nucleation of highly active CaCO3 accelerates the hydration kinetics of CWC3, generating more hydration products (such as Hc, Mc, and Ms), inducing denser pores, and ultimately contributing to the improved compressive strength. The carbonated waste exhibits the highest CO2 sequestration amount of 513.4 g/kg, underscoring the significant environmental sustainability of CWC3.
{"title":"Development of Carbonated Waste-Enhanced Calcined Clay Cement (CWC3) via Activated Carboaluminate Reaction: A Strategy toward Sustainable Engineering Materials","authors":"Xiaoyun Du,Zhiyuan Shao,Jun Chang,Kai Cui","doi":"10.1021/acssuschemeng.5c11743","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c11743","url":null,"abstract":"Limestone calcined clay cement (LC3) is widely recognized as a sustainable cementitious material. However, the low reactivity of natural limestone often limits the early carbon aluminate reaction and compromises the early compressive strength of LC3. This study proposes the preparation of highly active CaCO3 by carbonating SS, RCP, MS, and CS. The resulting product is then used to replace limestone and activate early carbon aluminate reactions in LC3. This strategy aims to develop a sustainable engineering material with high compressive strength and low CO2 emissions, referred to as carbonated waste calcined clay cement (CWC3). The results showed that compared with LC3, the compressive strength of CWC3 at 3 and 28 days increased by 19.7% and 10.8%, respectively, while the CO2 emissions and CO2 index decreased by 14.4% and 21.9%, respectively. The mechanism of early activation of the CWC3 carbon aluminate reaction includes two aspects: the crystallite grain size and crystallinity of CaCO3 in carbonated waste are much smaller and lower than those of CaCO3 in natural limestone with a polycrystalline crystal cluster morphology. This structure introduces a higher density of crystal defects, thereby enhancing chemical reactivity. CaCO3 crystal clusters and silica gel are interlaced in a carbonated waste particle, and the volcanic ash reaction of silica gel disperses the CaCO3 crystal clusters, thereby inducing more carbon aluminate reaction interfaces. In addition, the nucleation of highly active CaCO3 accelerates the hydration kinetics of CWC3, generating more hydration products (such as Hc, Mc, and Ms), inducing denser pores, and ultimately contributing to the improved compressive strength. The carbonated waste exhibits the highest CO2 sequestration amount of 513.4 g/kg, underscoring the significant environmental sustainability of CWC3.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"48 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147346687","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-04DOI: 10.1021/acssuschemeng.5c07420
Lena Nickel,Eric Schuler,Brian Rawls,Bart van den Bosch,Knut Stahl,Peter Moser,Li Shen
This article presents an ex ante life cycle assessment (LCA) of formic acid (FA) production on an industrial scale via the electrochemical reduction (ECR) of biogenic CO2 sourced from the incineration of wastewater sludge. Because renewable intermittent electricity is not suitable for continuous production and may be regulated by the EU, we model large-scale ECR-FA production using various power supply configurations, for example, by using the projected renewable electricity surplus for Germany in 2050 on an hourly resolution. The ECR-FA systems are compared to fossil-based FA production by using the 2020 and 2050 grid electricity mixes for Germany. Our LCA findings indicate that the most favorable system configuration in 2050 involves intermittent production with surplus renewable electricity, reducing GHG emissions by up to 83% relative to fossil FA, and also resulting in lower impacts than production with integrated battery storage or grid electricity. The main environmental impacts of ECR-FA production stem from the electricity demand in electrochemical conversion and purification. A cleaner electricity mix from 2020 to 2050 reduces climate impacts and nonrenewable energy use, yet it increases mineral and metal depletion. The materials used in the building of the electrolytic unit have a low environmental impact compared to the energy demands of electrolysis and purification. Future renewable grid power should be considered a constrained resource in the design of the upscaling of ECR technologies.
{"title":"Ex Ante Life Cycle Assessment of Industrial-Scale Electrochemical Reduction of CO2 to Formic Acid","authors":"Lena Nickel,Eric Schuler,Brian Rawls,Bart van den Bosch,Knut Stahl,Peter Moser,Li Shen","doi":"10.1021/acssuschemeng.5c07420","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c07420","url":null,"abstract":"This article presents an ex ante life cycle assessment (LCA) of formic acid (FA) production on an industrial scale via the electrochemical reduction (ECR) of biogenic CO2 sourced from the incineration of wastewater sludge. Because renewable intermittent electricity is not suitable for continuous production and may be regulated by the EU, we model large-scale ECR-FA production using various power supply configurations, for example, by using the projected renewable electricity surplus for Germany in 2050 on an hourly resolution. The ECR-FA systems are compared to fossil-based FA production by using the 2020 and 2050 grid electricity mixes for Germany. Our LCA findings indicate that the most favorable system configuration in 2050 involves intermittent production with surplus renewable electricity, reducing GHG emissions by up to 83% relative to fossil FA, and also resulting in lower impacts than production with integrated battery storage or grid electricity. The main environmental impacts of ECR-FA production stem from the electricity demand in electrochemical conversion and purification. A cleaner electricity mix from 2020 to 2050 reduces climate impacts and nonrenewable energy use, yet it increases mineral and metal depletion. The materials used in the building of the electrolytic unit have a low environmental impact compared to the energy demands of electrolysis and purification. Future renewable grid power should be considered a constrained resource in the design of the upscaling of ECR technologies.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"8 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147346688","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Aqueous zinc-ion batteries (AZIBs) represent a promising technology for grid-scale energy storage due to their intrinsic safety, environmental sustainability, and low cost. However, their practical implementation is hindered by severe anode instability issues, including uncontrollable dendrite growth and water-induced parasitic reactions. Here, we introduce sodium hexadecyl diphenyl ether disulfonate (SHDD) as a cost-effective, multifunctional electrolyte additive. The amphiphilic structure of SHDD– anion enables comprehensive interfacial regulation: the sulfonate groups facilitate Zn2+ desolvation while reducing water activity, and the adsorbed anions form a hydrophobic barrier that effectively suppresses the hydrogen evolution reaction (HER) and byproduct formation. Additionally, SHDD– anion adsorption induces vertically aligned and highly compact Zn2+ deposition along the Zn(100) crystal plane. Benefiting from this synergistic mechanism, the assembled Zn||Zn symmetric cells achieve exceptional cycling stability over 4200 h, while Zn||Cu half-cells maintain a 99.66% Coulombic efficiency. Furthermore, full cells with an NH4V4O10 cathode deliver 233.40 mAh g–1 at 1 A g–1 and retain 83% capacity after 600 cycles. Therefore, this study highlights the potential of molecular design in modulating crystal orientation and interface engineering for high-performance next-generation AZIBs.
水锌离子电池（azib）由于其固有的安全性、环境可持续性和低成本，代表了一种有前途的电网规模储能技术。然而，它们的实际实施受到严重的阳极不稳定性问题的阻碍，包括不可控的枝晶生长和水诱导的寄生反应。在这里，我们介绍了十六烷基二苯醚二磺酸钠（SHDD）作为一种具有成本效益的多功能电解质添加剂。SHDD -阴离子的两亲性结构实现了全面的界面调节：其中的硫酸盐基团有利于Zn2+的脱溶，同时降低了水活度，吸附的阴离子形成疏水屏障，有效抑制析氢反应（HER）和副产物的生成。此外，SHDD -阴离子吸附诱导沿Zn（100）晶面垂直排列且高度致密的Zn2+沉积。得益于这种协同机制，组装的Zn||Zn对称电池在4200 h内具有优异的循环稳定性，而Zn||Cu半电池则保持99.66%的库仑效率。此外，具有nh4v4010阴极的电池在1 A g-1下提供233.40 mAh g-1，并且在600次循环后保持83%的容量。因此，这项研究强调了分子设计在调制晶体取向和界面工程方面的潜力，以实现高性能的下一代azib。
{"title":"Molecular Engineering-Guided (100) Oriented Zinc Deposition of Anionic Surface-Active Additives for Ultrastable Zinc-Ion Batteries","authors":"Xin Huang,Zijing Yang,Guiying Yang,Xue Shu,Jinghua Liu,Xiang Wang,Yukun Wu,Zhuoshi Li,Jiaxin Guo,Rongying Zeng,Zhongliang Li,Liang Tan,Yue-Peng Cai","doi":"10.1021/acssuschemeng.5c13141","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c13141","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) represent a promising technology for grid-scale energy storage due to their intrinsic safety, environmental sustainability, and low cost. However, their practical implementation is hindered by severe anode instability issues, including uncontrollable dendrite growth and water-induced parasitic reactions. Here, we introduce sodium hexadecyl diphenyl ether disulfonate (SHDD) as a cost-effective, multifunctional electrolyte additive. The amphiphilic structure of SHDD– anion enables comprehensive interfacial regulation: the sulfonate groups facilitate Zn2+ desolvation while reducing water activity, and the adsorbed anions form a hydrophobic barrier that effectively suppresses the hydrogen evolution reaction (HER) and byproduct formation. Additionally, SHDD– anion adsorption induces vertically aligned and highly compact Zn2+ deposition along the Zn(100) crystal plane. Benefiting from this synergistic mechanism, the assembled Zn||Zn symmetric cells achieve exceptional cycling stability over 4200 h, while Zn||Cu half-cells maintain a 99.66% Coulombic efficiency. Furthermore, full cells with an NH4V4O10 cathode deliver 233.40 mAh g–1 at 1 A g–1 and retain 83% capacity after 600 cycles. Therefore, this study highlights the potential of molecular design in modulating crystal orientation and interface engineering for high-performance next-generation AZIBs.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"34 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147346701","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-04DOI: 10.1021/acssuschemeng.6c00171
Haijun Liu, Jiashun Zhang, Xinpeng Liu, Jiawen Wu, Junting Wu, Yan Gao, Xiaolong Wang, Mingyu Liu, Haijiang Wang
Optimizing the activity of alkaline hydrogen oxidation reaction (HOR) catalysts is pivotal for advancing the performance of alkaline fuel cells. However, the controversial modulation strategies for catalytic activity, along with the chasm between theoretical and experimental investigations, necessitate extensive trial-and-error experiments to maximize the alkaline HOR activity. Here, a comprehensive framework centered on theoretical kinetic analysis is introduced, integrating theoretical and experimental evaluation of alkaline HOR activity on Pt3M (M = Cr, Co, Pd, Sn, and Ir) catalysts, to address this challenge. This strategy not only validates electronic property and oxophilicity modulation factors of catalytic activity (with an upshift of the band center (εd) and increased oxophilicity compared to Pt), but also achieves an overlap ratio (Roverlap) of 92.94% to 99.39% between simulated and experimental polarization curves. Compared with oxophilicity modulation, the electronic property emerges as the dominant modulation factor governing alkaline HOR activity, as evidenced by their strong correlations with the free energy (Ea) of the rate-determining step and the exchange current density (i0), with degrees of correlation values of −0.98 and 0.98, respectively. This work bridges the chasm between theoretical and experimental investigation and advances the rational design and efficient synthesis of energy conversion catalysts.
{"title":"Enabling Direct Experimental Matched Activity Evaluation and Identification of a Dominant Modulation Factor via Theoretical Alkaline HOR Kinetic Analysis at the Catalyst/Electrolyte Interface","authors":"Haijun Liu, Jiashun Zhang, Xinpeng Liu, Jiawen Wu, Junting Wu, Yan Gao, Xiaolong Wang, Mingyu Liu, Haijiang Wang","doi":"10.1021/acssuschemeng.6c00171","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c00171","url":null,"abstract":"Optimizing the activity of alkaline hydrogen oxidation reaction (HOR) catalysts is pivotal for advancing the performance of alkaline fuel cells. However, the controversial modulation strategies for catalytic activity, along with the chasm between theoretical and experimental investigations, necessitate extensive trial-and-error experiments to maximize the alkaline HOR activity. Here, a comprehensive framework centered on theoretical kinetic analysis is introduced, integrating theoretical and experimental evaluation of alkaline HOR activity on Pt<sub>3</sub>M (M = Cr, Co, Pd, Sn, and Ir) catalysts, to address this challenge. This strategy not only validates electronic property and oxophilicity modulation factors of catalytic activity (with an upshift of the band center (ε<sub>d</sub>) and increased oxophilicity compared to Pt), but also achieves an overlap ratio (<i>R</i><sub>overlap</sub>) of 92.94% to 99.39% between simulated and experimental polarization curves. Compared with oxophilicity modulation, the electronic property emerges as the dominant modulation factor governing alkaline HOR activity, as evidenced by their strong correlations with the free energy (<i>E</i><sub>a</sub>) of the rate-determining step and the exchange current density (<i>i</i><sub>0</sub>), with degrees of correlation values of −0.98 and 0.98, respectively. This work bridges the chasm between theoretical and experimental investigation and advances the rational design and efficient synthesis of energy conversion catalysts.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"17 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147358817","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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