Pub Date : 2026-02-10DOI: 10.1016/j.cej.2026.174004
Yanbei Liu, Ruoming Wang, Xiao Lin, Taimoor Raza, Muhammad Qadeer, Wen-Feng Lin, Sining Yun
Compared with conventional ionic electrolyte-based solid oxide fuel cells, mixed ionic electronic conductor (MIEC) electrolytes enable high power at relatively low temperatures. Here, we design a hybrid ionic-electronic conductor electrolyte based on p-n heterojunctions: a layered perovskite-type high-entropy oxide (La0.2Pr0.2Nd0.2Sm0.2Sr0.2)2CuO4 (HEO) as the p-type semiconductor combined with the n-type fluorite Nd0.05Ce0.95O2-δ (NDC). This study marks their first application in fuel-cell electrolyte composites. The multielemental composition of the HEO tailors the electronic structure to stabilize the interfacial charge dynamics and enhance ionic conduction via lattice disorder, which reduces the migration barriers. Integration with NDC induces band bending at heterogeneous interfaces and synergistically improves the carrier dynamics. In this heterostructure, the built-in electric field generated by the Fermi-level alignment suppresses electron penetration while driving ion/proton transport; concurrently, interfacial charge compensation induces oxygen vacancy formation, synergistically enhancing superionic conduction. Consequently, systematic optimization of HEO-NDC mass ratios combined with multiscale characterization identifies the 3HEO:7NDC composite as optimal, achieving a peak power density of 995.3 mW cm−2 with an open-circuit voltage (OCV) of 1.067 V at 550 °C and approximately 50-h stability. This study demonstrates a new strategy for the development of HEO-based hybrid conductor electrolytes.
{"title":"Driving superionic transport in high-entropy oxide/fluorite heterostructure electrolytes for boosting fuel cell performance","authors":"Yanbei Liu, Ruoming Wang, Xiao Lin, Taimoor Raza, Muhammad Qadeer, Wen-Feng Lin, Sining Yun","doi":"10.1016/j.cej.2026.174004","DOIUrl":"https://doi.org/10.1016/j.cej.2026.174004","url":null,"abstract":"Compared with conventional ionic electrolyte-based solid oxide fuel cells, mixed ionic electronic conductor (MIEC) electrolytes enable high power at relatively low temperatures. Here, we design a hybrid ionic-electronic conductor electrolyte based on p-n heterojunctions: a layered perovskite-type high-entropy oxide (La<ce:inf loc=\"post\">0.2</ce:inf>Pr<ce:inf loc=\"post\">0.2</ce:inf>Nd<ce:inf loc=\"post\">0.2</ce:inf>Sm<ce:inf loc=\"post\">0.2</ce:inf>Sr<ce:inf loc=\"post\">0.2</ce:inf>)<ce:inf loc=\"post\">2</ce:inf>CuO<ce:inf loc=\"post\">4</ce:inf> (HEO) as the p-type semiconductor combined with the n-type fluorite Nd<ce:inf loc=\"post\">0.05</ce:inf>Ce<ce:inf loc=\"post\">0.95</ce:inf>O<ce:inf loc=\"post\">2-δ</ce:inf> (NDC). This study marks their first application in fuel-cell electrolyte composites. The multielemental composition of the HEO tailors the electronic structure to stabilize the interfacial charge dynamics and enhance ionic conduction via lattice disorder, which reduces the migration barriers. Integration with NDC induces band bending at heterogeneous interfaces and synergistically improves the carrier dynamics. In this heterostructure, the built-in electric field generated by the Fermi-level alignment suppresses electron penetration while driving ion/proton transport; concurrently, interfacial charge compensation induces oxygen vacancy formation, synergistically enhancing superionic conduction. Consequently, systematic optimization of HEO-NDC mass ratios combined with multiscale characterization identifies the 3HEO:7NDC composite as optimal, achieving a peak power density of 995.3 mW cm<ce:sup loc=\"post\">−2</ce:sup> with an open-circuit voltage (OCV) of 1.067 V at 550 °C and approximately 50-h stability. This study demonstrates a new strategy for the development of HEO-based hybrid conductor electrolytes.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"99 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153161","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-10DOI: 10.1016/j.cej.2026.174034
Jong Chan Choi, Da-Eun Hyun, Jae Sol Sim, Inuk Lee, Yun Chan Kang
Zn metal anodes are promising for rechargeable aqueous zinc-ion batteries; however, practical deployment requires the use of thin Zn layers to preserve the energy density and suppress dendrite growth and corrosion driven by the hydrogen evolution reaction (HER). Herein, an ultrathin Zn anode (~9 μm) is constructed with a zincophilic ZnSe layer with a thickness of approximately 100 nm. Electroplating is introduced to form the Zn anode, the deposition time is adjusted to control the thickness, and the resulting thin layer exhibits improved mechanical flexibility. Density functional theory and COMSOL analyses indicate that the ZnSe interphase facilitates interfacial supply of Zn2+, consistent with the observed uniform plating/stripping and low interfacial resistance. ZnSe treatment limits the direct contact between the electrolyte and Zn metal and increases the Zn (002) texture, thereby suppressing HER-induced corrosion. Consequently, when paired with V2O5 cathodes under a low N/P ratio of 2.6 in full cells, the anode maintains a capacity of 160 mAh g−1 for more than 1500 cycles at 5 A g−1. In contrast to surface treatment of thick commercial Zn foil, this scalable interfacial engineering strategy for ultrathin Zn metal anodes enables high energy density and long cycle life in practical cells.
锌金属阳极在可充电水性锌离子电池中具有广阔的应用前景；然而，实际部署需要使用薄锌层来保持能量密度，抑制析氢反应（HER）驱动的枝晶生长和腐蚀。本文用厚度约为100 nm的亲锌ZnSe层构建了超薄Zn阳极（~9 μm）。采用电镀法制备锌阳极，通过调整沉积时间来控制锌阳极的厚度，得到的锌阳极薄层具有更好的机械柔韧性。密度泛函理论和COMSOL分析表明，ZnSe界面相有利于Zn2+的界面供应，与观察到的均匀镀/剥离和低界面电阻一致。ZnSe处理限制了电解液与Zn金属之间的直接接触，增加了Zn（002）织构，从而抑制了her引起的腐蚀。因此，当在全电池中与低N/P比为2.6的V2O5阴极配对时，阳极在5a g−1下保持超过1500次 循环的容量为160 mAh g−1。与厚商业锌箔的表面处理相比，这种用于超薄锌金属阳极的可扩展界面工程策略可在实际电池中实现高能量密度和长循环寿命。
{"title":"Zincophilic ultrathin Zn metal anode enabling uniform deposition and corrosion suppression in aqueous zinc ion batteries","authors":"Jong Chan Choi, Da-Eun Hyun, Jae Sol Sim, Inuk Lee, Yun Chan Kang","doi":"10.1016/j.cej.2026.174034","DOIUrl":"https://doi.org/10.1016/j.cej.2026.174034","url":null,"abstract":"Zn metal anodes are promising for rechargeable aqueous zinc-ion batteries; however, practical deployment requires the use of thin Zn layers to preserve the energy density and suppress dendrite growth and corrosion driven by the hydrogen evolution reaction (HER). Herein, an ultrathin Zn anode (~9 μm) is constructed with a zincophilic ZnSe layer with a thickness of approximately 100 nm. Electroplating is introduced to form the Zn anode, the deposition time is adjusted to control the thickness, and the resulting thin layer exhibits improved mechanical flexibility. Density functional theory and COMSOL analyses indicate that the ZnSe interphase facilitates interfacial supply of Zn<ce:sup loc=\"post\">2+</ce:sup>, consistent with the observed uniform plating/stripping and low interfacial resistance. ZnSe treatment limits the direct contact between the electrolyte and Zn metal and increases the Zn (002) texture, thereby suppressing HER-induced corrosion. Consequently, when paired with V<ce:inf loc=\"post\">2</ce:inf>O<ce:inf loc=\"post\">5</ce:inf> cathodes under a low N/P ratio of 2.6 in full cells, the anode maintains a capacity of 160 mAh g<ce:sup loc=\"post\">−1</ce:sup> for more than 1500 cycles at 5 A g<ce:sup loc=\"post\">−1</ce:sup>. In contrast to surface treatment of thick commercial Zn foil, this scalable interfacial engineering strategy for ultrathin Zn metal anodes enables high energy density and long cycle life in practical cells.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"32 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153164","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-10DOI: 10.1016/j.cej.2026.173927
Qiangsong Jiang, Zechang Wei, De Li, Yongning Tu, Xiaohong Yu, Zhinan Wang, Hong Lei
Developing aqueous biomass adhesives that can simultaneously achieve long open assembly time (high water retention) and exceptional cured water resistance remains a challenge in wood composites engineering. Herein, a hierarchical hydro-confinement strategy was proposed to fabricate a water resistant soybean flour (SF) adhesive with excellent water retention performance and multi-functionality. The architecture of adhesive integrates oxidized sucrose as a molecular anchor, aminated nano-silica as a rigid tortuous barrier, and phytic acid as an ionic densifier. Specifically, in the liquid state, the system acts as a water confinement effect which converts free water into thermodynamically stable bound water via abundant hydrogen bonding sites and physical obstruction, retaining over 74% of moisture after 24 h and extending the open assembly time to 60 min without compromising bonding efficacy. Upon hot-pressing, this hydrophilic network transforms into a dense, hydrophobic cross-linked structure via Schiff base reactions and ionic coordination. The optimized adhesive achieves a high wet shear strength of 1.52 MPa and retains 1.18 MPa after immersion in water for 30 days. Furthermore, the incorporation of the organic-inorganic hybrid framework improves flame retardancy and suppresses visible mold growth under the tested conditions. This work provides a facile and practical structural densification method for advancing high-performance bio-based adhesives.
{"title":"Constructing a hierarchical hydro-confinement network for strong, water-retaining, and multifunctional soybean flour adhesives","authors":"Qiangsong Jiang, Zechang Wei, De Li, Yongning Tu, Xiaohong Yu, Zhinan Wang, Hong Lei","doi":"10.1016/j.cej.2026.173927","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173927","url":null,"abstract":"Developing aqueous biomass adhesives that can simultaneously achieve long open assembly time (high water retention) and exceptional cured water resistance remains a challenge in wood composites engineering. Herein, a hierarchical hydro-confinement strategy was proposed to fabricate a water resistant soybean flour (SF) adhesive with excellent water retention performance and multi-functionality. The architecture of adhesive integrates oxidized sucrose as a molecular anchor, aminated nano-silica as a rigid tortuous barrier, and phytic acid as an ionic densifier. Specifically, in the liquid state, the system acts as a water confinement effect which converts free water into thermodynamically stable bound water via abundant hydrogen bonding sites and physical obstruction, retaining over 74% of moisture after 24 h and extending the open assembly time to 60 min without compromising bonding efficacy. Upon hot-pressing, this hydrophilic network transforms into a dense, hydrophobic cross-linked structure via Schiff base reactions and ionic coordination. The optimized adhesive achieves a high wet shear strength of 1.52 MPa and retains 1.18 MPa after immersion in water for 30 days. Furthermore, the incorporation of the organic-inorganic hybrid framework improves flame retardancy and suppresses visible mold growth under the tested conditions. This work provides a facile and practical structural densification method for advancing high-performance bio-based adhesives.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"317 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153174","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-10DOI: 10.1016/j.cej.2026.173120
Bin Liu, Jiashen Hu, Zitong Zhao, Long Yang, Chengcheng Su, Nan Yan, Tiehan Zhang, Rongjiao Li, Huajiang Dong, Lu Liu
Drug-resistant bacteria pose a serious threat to human health, making the urgent development of alternative treatments essential. Photodynamic therapy is an effective antibacterial approach, with the properties of its photocatalyst being one of the most important factors. In this study, different templates are designed to control the defect types of SnS during synthesis, resulting in two types of samples, SnS-1 and SnS-2, which predominantly feature VSnSSSn and VSnSn defects, respectively. The theoretical calculation through the first principle and experimental information reveal that SnS-1, with VSnSSSn defects, can generate more reactive oxygen species (ROS) due to better absorption of O2 molecules, H2O molecules, and LPS, along with a narrower bandgap, leading to higher inactivation of E. coli compared to SnS-2 with VSnSn defects. Therefore, defect engineering presents a promising approach for enhancing the inactivation of drug-resistant bacteria through photodynamic therapy.
{"title":"Tuning the electronic structure of SnS for efficient inactivation of E. coli relying on defect engineering","authors":"Bin Liu, Jiashen Hu, Zitong Zhao, Long Yang, Chengcheng Su, Nan Yan, Tiehan Zhang, Rongjiao Li, Huajiang Dong, Lu Liu","doi":"10.1016/j.cej.2026.173120","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173120","url":null,"abstract":"Drug-resistant bacteria pose a serious threat to human health, making the urgent development of alternative treatments essential. Photodynamic therapy is an effective antibacterial approach, with the properties of its photocatalyst being one of the most important factors. In this study, different templates are designed to control the defect types of SnS during synthesis, resulting in two types of samples, SnS-1 and SnS-2, which predominantly feature VSnSSSn and VSnSn defects, respectively. The theoretical calculation through the first principle and experimental information reveal that SnS-1, with VSnSSSn defects, can generate more reactive oxygen species (ROS) due to better absorption of O<ce:inf loc=\"post\">2</ce:inf> molecules, H<ce:inf loc=\"post\">2</ce:inf>O molecules, and LPS, along with a narrower bandgap, leading to higher inactivation of <ce:italic>E. coli</ce:italic> compared to SnS-2 with VSnSn defects. Therefore, defect engineering presents a promising approach for enhancing the inactivation of drug-resistant bacteria through photodynamic therapy.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"317 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153187","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Gouty arthritis (GA), caused by monosodium urate crystal deposition in the context of persistent hyperuricemia, remains difficult to treat due to the inability of conventional therapies to simultaneously control uric acid (UA) levels, oxidative stress, and inflammation. To overcome this, we develop a biomimetic nanozyme composed of AuPt bimetallic nanozymes cloaked with erythrocyte membrane (AuPt@EM). It integrates prolonged circulation with cascade enzyme activities to achieve systemic UA reduction, local crystal clearance, and modulation of the inflammatory hypoxic microenvironment. AuPt@EM exhibits superoxide dismutase-like and catalase-like activities, efficiently scavenging ROS and generating oxygen, thereby amplifying its uricase-like activity to sustainably reduce UA. This nanozyme reduces ROS, suppresses the PI3K/AKT/HIF-1α pathway, and promotes HIF-1α degradation, which reprograms macrophages from the pro-inflammatory M1 phenotype toward the anti-inflammatory M2 phenotype. In vivo, AuPt@EM facilitates crystal clearance, alleviates joint inflammation, and preserves cartilage integrity. Moreover, it restores systemic immune balance by elevating IL-10 while decreasing IL-1β and IL-6. This study establishes an integrated therapeutic paradigm that combines UA level control, crystal dissolution, and inflammatory hypoxic microenvironment modulation, offering a promising strategy for precise and effective intervention in hyperuricemia and gouty arthritis.
{"title":"A biomimetic nanozyme enabling prolonged blood circulation for precise Theranostics in hyperuricemia and gouty arthritis","authors":"Lujie Yu, Qin Liu, Shutong Wu, Jian Zhang, Lin Chen, Huifang Hao, Mingxin Zhao, Chunmei Jiang, Weiwei Zhang, Ziliang Zheng, Ruiping Zhang","doi":"10.1016/j.cej.2026.173944","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173944","url":null,"abstract":"Gouty arthritis (GA), caused by monosodium urate crystal deposition in the context of persistent hyperuricemia, remains difficult to treat due to the inability of conventional therapies to simultaneously control uric acid (UA) levels, oxidative stress, and inflammation. To overcome this, we develop a biomimetic nanozyme composed of AuPt bimetallic nanozymes cloaked with erythrocyte membrane (AuPt@EM). It integrates prolonged circulation with cascade enzyme activities to achieve systemic UA reduction, local crystal clearance, and modulation of the inflammatory hypoxic microenvironment. AuPt@EM exhibits superoxide dismutase-like and catalase-like activities, efficiently scavenging ROS and generating oxygen, thereby amplifying its uricase-like activity to sustainably reduce UA. This nanozyme reduces ROS, suppresses the PI3K/AKT/HIF-1α pathway, and promotes HIF-1α degradation, which reprograms macrophages from the pro-inflammatory M1 phenotype toward the anti-inflammatory M2 phenotype. In vivo, AuPt@EM facilitates crystal clearance, alleviates joint inflammation, and preserves cartilage integrity. Moreover, it restores systemic immune balance by elevating IL-10 while decreasing IL-1β and IL-6. This study establishes an integrated therapeutic paradigm that combines UA level control, crystal dissolution, and inflammatory hypoxic microenvironment modulation, offering a promising strategy for precise and effective intervention in hyperuricemia and gouty arthritis.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"73 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146186","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-10DOI: 10.1016/j.cej.2026.173601
Leila Shahriari, Tyrus Antonson, Sang Eon Han, Sang M. Han, Maryam Hojati, Sungjin Kim
Carbon dioxide (CO2) mineralization offers a promising strategy to convert waste carbon into valuable carbonate feedstocks. Practical industrial implementation, however, requires precise reaction engineering to optimize efficiency while controlling particle morphology and polymorphism. We present a systematically designed reaction-engineering framework that elucidates the mechanistic controls governing catechol-mediated CO2 mineralization, inspired by biomineralization processes in marine environments, enabling tunable control over calcium carbonate (CaCO3) phase, morphology, and particle size. Within this framework, we integrate tannic acid (TA) and ultrasonic irradiation to enhance reaction kinetics and CO2 utilization. The combined use of TA and ultrasonication enhances the product yield by up to ∼300% compared with the control without polyphenol and ultrasonication. The improvement is attributed to the Ca-binding of TA, which accelerates nucleation and stabilizes the metastable vaterite phase, along with ultrasound-induced improvements in CO2 dissolution and mass transfer. Under these conditions, uniform spherical vaterite particles with diameters of 1–2 μm are produced as a result of intensified nucleation, enhanced CO2 dissolution, and the generation of smaller CO2 bubbles that serve as nucleation templates. These findings highlight a bioinspired organic-inorganic reaction engineering framework for scalable, efficient CO2 utilization toward sustainable manufacturing applications.
{"title":"Bioinspired reaction engineering of CO2 mineralization assisted by tannic acid and ultrasonication","authors":"Leila Shahriari, Tyrus Antonson, Sang Eon Han, Sang M. Han, Maryam Hojati, Sungjin Kim","doi":"10.1016/j.cej.2026.173601","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173601","url":null,"abstract":"Carbon dioxide (CO<ce:inf loc=\"post\">2</ce:inf>) mineralization offers a promising strategy to convert waste carbon into valuable carbonate feedstocks. Practical industrial implementation, however, requires precise reaction engineering to optimize efficiency while controlling particle morphology and polymorphism. We present a systematically designed reaction-engineering framework that elucidates the mechanistic controls governing catechol-mediated CO<ce:inf loc=\"post\">2</ce:inf> mineralization, inspired by biomineralization processes in marine environments, enabling tunable control over calcium carbonate (CaCO<ce:inf loc=\"post\">3</ce:inf>) phase, morphology, and particle size. Within this framework, we integrate tannic acid (TA) and ultrasonic irradiation to enhance reaction kinetics and CO<ce:inf loc=\"post\">2</ce:inf> utilization. The combined use of TA and ultrasonication enhances the product yield by up to ∼300% compared with the control without polyphenol and ultrasonication. The improvement is attributed to the Ca-binding of TA, which accelerates nucleation and stabilizes the metastable vaterite phase, along with ultrasound-induced improvements in CO<ce:inf loc=\"post\">2</ce:inf> dissolution and mass transfer. Under these conditions, uniform spherical vaterite particles with diameters of 1–2 μm are produced as a result of intensified nucleation, enhanced CO<ce:inf loc=\"post\">2</ce:inf> dissolution, and the generation of smaller CO<ce:inf loc=\"post\">2</ce:inf> bubbles that serve as nucleation templates. These findings highlight a bioinspired organic-inorganic reaction engineering framework for scalable, efficient CO<ce:inf loc=\"post\">2</ce:inf> utilization toward sustainable manufacturing applications.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"244 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146711","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-10DOI: 10.1016/j.cej.2026.173952
Feike Zhang, Jun Wang, Guixi Wang, Xiaoke Li, Weikun Ren, Jinghua Yang, Ruilong Liu, Shiyu Wang, Kang Ji, Shuyun Yao, Yingjie Ji, Jingyu Wu, Wanlong Bai, Zhiyu Yang, Yi-Ming Yan
Formate represents a promising liquid hydrogen carrier for advancing carbon neutrality goals while serving as a key intermediate in closed-loop carbon cycling systems. Despite their resistance to carbonaceous poisoning that plagues Pt catalysts, Pd-based electrocatalysts for formate oxidation reaction (FOR) suffer from performance degradation due to accumulating hydrogen intermediates (H*) that block active sites. Here, we report a MoS₂-supported Pd nanocatalyst (Pd/MoS₂/C) featuring bidirectional interfacial electronic interactions that fundamentally address H* poisoning through facilitated hydrogen spillover. This engineered interface establishes a two-way electronic communication: electron transfer from MoS₂ to Pd induces a downshift in the Pd d-band center, weakening Pd–H* bonds and promoting H* desorption, while simultaneously, Pd catalyzes a 2H-to-1 T phase transition in MoS₂, enhancing its electronic conductivity and hydrogen-hosting capability. The resulting catalyst achieves an exceptional mass activity of 7.92 A mgPd−1 for FOR—5.18-fold higher than commercial Pd/C. Through combined spectroscopic analyses and density functional theory calculations, we demonstrate that this bidirectional electronic coupling creates a self-sustaining hydrogen spillover pathway functioning as a hydrogen diode that continuously regenerates active Pd sites during catalysis. Our findings establish bidirectional interface engineering as a powerful approach for overcoming hydrogen-induced deactivation in Pd-based systems and highlight the critical role of phase-tunable 2D materials in designing high-performance electrocatalysts for sustainable energy conversion.
甲酸盐是一种很有前途的液氢载体，可以促进碳中和目标的实现，同时也是闭环碳循环系统的关键中间体。尽管铂催化剂具有抗碳中毒的能力，但甲酸酯氧化反应（for）的钯基电催化剂由于积累氢中间体（H*）阻塞活性位点而导致性能下降。在这里，我们报道了一种具有双向界面电子相互作用的MoS₂负载的Pd纳米催化剂（Pd/MoS₂/C），该催化剂通过促进氢溢出从根本上解决了氢中毒问题。该工程界面建立了双向电子通信：从MoS 2到Pd的电子转移引起Pd d带中心的下移，减弱Pd - H*键并促进H*解吸，同时，Pd催化MoS 2的2h -1 T相变，增强其电子导电性和载氢能力。所得催化剂的质量活性为7.92 A mgPd−1，比商用Pd/C高5.18倍。通过结合光谱分析和密度泛函理论计算，我们证明了这种双向电子耦合创造了一个自我维持的氢溢出途径，作为一个氢二极管，在催化过程中不断再生活性Pd位点。我们的研究结果确立了双向界面工程是克服pd基体系中氢诱导失活的有力方法，并强调了相可调二维材料在设计高性能电催化剂以实现可持续能量转换方面的关键作用。
{"title":"Bidirectionally interfacial electronic interactions in Pd/MoS₂ enable efficient formate oxidation through facilitated hydrogen spillover","authors":"Feike Zhang, Jun Wang, Guixi Wang, Xiaoke Li, Weikun Ren, Jinghua Yang, Ruilong Liu, Shiyu Wang, Kang Ji, Shuyun Yao, Yingjie Ji, Jingyu Wu, Wanlong Bai, Zhiyu Yang, Yi-Ming Yan","doi":"10.1016/j.cej.2026.173952","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173952","url":null,"abstract":"Formate represents a promising liquid hydrogen carrier for advancing carbon neutrality goals while serving as a key intermediate in closed-loop carbon cycling systems. Despite their resistance to carbonaceous poisoning that plagues Pt catalysts, Pd-based electrocatalysts for formate oxidation reaction (FOR) suffer from performance degradation due to accumulating hydrogen intermediates (H*) that block active sites. Here, we report a MoS₂-supported Pd nanocatalyst (Pd/MoS₂/C) featuring bidirectional interfacial electronic interactions that fundamentally address H* poisoning through facilitated hydrogen spillover. This engineered interface establishes a two-way electronic communication: electron transfer from MoS₂ to Pd induces a downshift in the Pd d-band center, weakening Pd–H* bonds and promoting H* desorption, while simultaneously, Pd catalyzes a 2H-to-1 T phase transition in MoS₂, enhancing its electronic conductivity and hydrogen-hosting capability. The resulting catalyst achieves an exceptional mass activity of 7.92 A mg<ce:inf loc=\"post\">Pd</ce:inf><ce:sup loc=\"post\">−1</ce:sup> for FOR—5.18-fold higher than commercial Pd/C. Through combined spectroscopic analyses and density functional theory calculations, we demonstrate that this bidirectional electronic coupling creates a self-sustaining hydrogen spillover pathway functioning as a hydrogen diode that continuously regenerates active Pd sites during catalysis. Our findings establish bidirectional interface engineering as a powerful approach for overcoming hydrogen-induced deactivation in Pd-based systems and highlight the critical role of phase-tunable 2D materials in designing high-performance electrocatalysts for sustainable energy conversion.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"89 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146709","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Phase change materials (PCMs) have demonstrated substantial potential in multiple energy storage applications. However, critical obstacles remain, including PCM leakage in liquid state, structural failure under external loads, and the lack of photo-/magnetothermal storage capability. Inspired by natural honeycomb structure, this work presents a one-step hydrothermal method of in situ growing Ni3S2 nanosheet arrays on nickel foam (Ni foam), subsequently encapsulating polyethylene glycol (PEG) to fabricate multifunctional PCM composites. Benefiting from the honeycomb-like architectures and the hydrogen bonding interactions between Ni3S2 nanosheets and PEG chains, the Ni@Ni3S2/PEG composite maintains excellent shape stability even after 8 h of intensive thermal cycling. Notably, the composite exhibits superior mechanical properties at both ambient temperature and above the melting point, with compressive strength enhanced by 430% to 780% compared to pristine PEG, alongside minimal leakage. Comprehensive analysis reveals that Ni3S2 nanosheets serve as heterogeneous nucleation sites, effectively reducing the crystallization activation energy of PEG from 160.3 kJ/mol to 125.6 kJ/mol. Simultaneously, the geometric confinement effect of Ni3S2 nanosheets guides the ordered arrangement of PEG chains and facilitates their rapid crystallization. Moreover, the composite successfully integrates magnetic-induced heating and photothermal conversion capabilities. Broadband light absorption (95.2%) is achieved by synergistically enhancing multiple scattering through a three-dimensional (3D) Ni foam porous structure integrated with Ni3S2 nanosheet arrays. A constructed solar-powered electricity generation device achieves a sustained current output of 168.35 mA. This work provides a facile design strategy for realizing synergistic enhancement of encapsulation performance, thermal storage density, and photothermal conversion in porous foam-based PCMs.
{"title":"Honeycomb-inspired Ni/Ni3S2 foam stabilizing phase change composites for multiple energy storage","authors":"Zi-jie Huang, Qin Wang, Zi-cheng Tang, Hao-hao Song, Jing-hui Yang, De-xiang Sun, Xiao-dong Qi, Yong Wang","doi":"10.1016/j.cej.2026.174023","DOIUrl":"https://doi.org/10.1016/j.cej.2026.174023","url":null,"abstract":"Phase change materials (PCMs) have demonstrated substantial potential in multiple energy storage applications. However, critical obstacles remain, including PCM leakage in liquid state, structural failure under external loads, and the lack of photo-/magnetothermal storage capability. Inspired by natural honeycomb structure, this work presents a one-step hydrothermal method of in situ growing Ni<ce:inf loc=\"post\">3</ce:inf>S<ce:inf loc=\"post\">2</ce:inf> nanosheet arrays on nickel foam (Ni foam), subsequently encapsulating polyethylene glycol (PEG) to fabricate multifunctional PCM composites. Benefiting from the honeycomb-like architectures and the hydrogen bonding interactions between Ni<ce:inf loc=\"post\">3</ce:inf>S<ce:inf loc=\"post\">2</ce:inf> nanosheets and PEG chains, the Ni@Ni<ce:inf loc=\"post\">3</ce:inf>S<ce:inf loc=\"post\">2</ce:inf>/PEG composite maintains excellent shape stability even after 8 h of intensive thermal cycling. Notably, the composite exhibits superior mechanical properties at both ambient temperature and above the melting point, with compressive strength enhanced by 430% to 780% compared to pristine PEG, alongside minimal leakage. Comprehensive analysis reveals that Ni<ce:inf loc=\"post\">3</ce:inf>S<ce:inf loc=\"post\">2</ce:inf> nanosheets serve as heterogeneous nucleation sites, effectively reducing the crystallization activation energy of PEG from 160.3 kJ/mol to 125.6 kJ/mol. Simultaneously, the geometric confinement effect of Ni<ce:inf loc=\"post\">3</ce:inf>S<ce:inf loc=\"post\">2</ce:inf> nanosheets guides the ordered arrangement of PEG chains and facilitates their rapid crystallization. Moreover, the composite successfully integrates magnetic-induced heating and photothermal conversion capabilities. Broadband light absorption (95.2%) is achieved by synergistically enhancing multiple scattering through a three-dimensional (3D) Ni foam porous structure integrated with Ni<ce:inf loc=\"post\">3</ce:inf>S<ce:inf loc=\"post\">2</ce:inf> nanosheet arrays. A constructed solar-powered electricity generation device achieves a sustained current output of 168.35 mA. This work provides a facile design strategy for realizing synergistic enhancement of encapsulation performance, thermal storage density, and photothermal conversion in porous foam-based PCMs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"13 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153165","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-10DOI: 10.1016/j.cej.2026.174039
Qiushi Chen, Xuzhong Gong, Junhao Liu, Zhi Wang
Micron silicon has long suffered from poor ion transport capability despite the potential as a reliable anode material for next-generation lithium-ion batteries. In this work, we present a novel strategy that leverages the inherent Al impurities in waste photovoltaic cell wafers to fabricate LiAlO₂-coated micron silicon anode via electrothermal shock process. The LiAlO₂ layer can effectively mitigate silicon's volume expansion through mechanical constraint, while the intense thermal gradient generated during electrothermal shock induces abundant oxygen vacancies in the coating, thereby facilitating rapid lithium-ion transport. The asymmetric bonding at the Si/LiAlO₂ interface, together with the work function difference between the two materials, enhances lithium-ion transport across the interface. Partially pre-lithiated silicon during the synthesis of LiAlO2 and stable SEI formation achieve a high ICE of 91%. Long-term cycling tests demonstrate a stable capacity over 2300 mAh g−1 after 300 cycles at 0.5 A g−1, with a retention of 92%, and impressive rate capability with over 750 mAh g−1 maintained after 1000 cycles at 5 A g−1. Full cell with μm-Si@LAO anode and commercial NCM811 cathode deliver an energy density of over 480 Wh kg−1 at 0.5C. This work presents a promising strategy for developing high-performance micron silicon anodes with enhanced lithium-ion transport properties.
尽管作为下一代锂离子电池可靠的负极材料，微米硅长期以来一直受到离子传输能力差的困扰。在这项工作中，我们提出了一种新的策略，利用废弃光伏电池晶片中固有的Al杂质，通过电热冲击工艺制造LiAlO 2涂层的微米硅阳极。LiAlO₂层可以通过机械约束有效地减缓硅的体积膨胀，而电热冲击过程中产生的强烈热梯度会在涂层中产生丰富的氧空位，从而促进锂离子的快速传输。Si/LiAlO 2界面上的不对称键合以及两种材料之间的功函数差异增强了锂离子在界面上的输运。在LiAlO2合成过程中，部分预锂化硅和稳定的SEI形成实现了91%的高ICE。长期骑自行车测试演示一个稳定的容量超过2300 mAh g−1 300年后 周期在0.5 g−1,保留92%,令人印象深刻的速度能力超过750 mAh g−1 1000年后保持 周期在5 g−1。具有μm-Si@LAO阳极和商用NCM811阴极的全电池在0.5℃下提供超过480 Wh kg−1的能量密度。这项工作为开发具有增强锂离子输运性能的高性能微米硅阳极提供了一个有前途的策略。
{"title":"Surface-engineered micron silicon for lithium-ion battery anode with enhanced ion transport","authors":"Qiushi Chen, Xuzhong Gong, Junhao Liu, Zhi Wang","doi":"10.1016/j.cej.2026.174039","DOIUrl":"https://doi.org/10.1016/j.cej.2026.174039","url":null,"abstract":"Micron silicon has long suffered from poor ion transport capability despite the potential as a reliable anode material for next-generation lithium-ion batteries. In this work, we present a novel strategy that leverages the inherent Al impurities in waste photovoltaic cell wafers to fabricate LiAlO₂-coated micron silicon anode via electrothermal shock process. The LiAlO₂ layer can effectively mitigate silicon's volume expansion through mechanical constraint, while the intense thermal gradient generated during electrothermal shock induces abundant oxygen vacancies in the coating, thereby facilitating rapid lithium-ion transport. The asymmetric bonding at the Si/LiAlO₂ interface, together with the work function difference between the two materials, enhances lithium-ion transport across the interface. Partially pre-lithiated silicon during the synthesis of LiAlO<ce:inf loc=\"post\">2</ce:inf> and stable SEI formation achieve a high ICE of 91%. Long-term cycling tests demonstrate a stable capacity over 2300 mAh g<ce:sup loc=\"post\">−1</ce:sup> after 300 cycles at 0.5 A g<ce:sup loc=\"post\">−1</ce:sup>, with a retention of 92%, and impressive rate capability with over 750 mAh g<ce:sup loc=\"post\">−1</ce:sup> maintained after 1000 cycles at 5 A g<ce:sup loc=\"post\">−1</ce:sup>. Full cell with μm-Si@LAO anode and commercial NCM811 cathode deliver an energy density of over 480 Wh kg<ce:sup loc=\"post\">−1</ce:sup> at 0.5C. This work presents a promising strategy for developing high-performance micron silicon anodes with enhanced lithium-ion transport properties.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"5 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153176","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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