Chemical Engineering Journal最新文献

{"title":"A dual-factor-gated DNA nanomachine enables spatially controlled microRNA imaging with improved tumor specificity","authors":"Chang Liu, Lie Li, Baozhu Hu, Yu Wang, Heng Zhou, Jianwei Jiao, Shoufeng Wang, Jin Jiao","doi":"10.1016/j.cej.2026.182737","DOIUrl":"https://doi.org/10.1016/j.cej.2026.182737","url":null,"abstract":"The precise imaging of microRNA (miRNA) in living systems is essential for early cancer diagnosis and therapeutic evaluation. However, existing miRNA imaging approaches are often hampered by low spatial resolution and limited tumor specificity. Here, we report a dual-factor-gated DNA nanomachine (DDN) for spatially controlled imaging of miRNA with high tumor specificity. Specifically, the sensing function of DDN is blocked through the elaborate implementation of an adenosine triphosphate (ATP) aptamer and an abasic site, which can be activated by two endogenous tumor-associated factors (ATP and apurinic/apyrimidinic endonuclease 1), thus achieving tumor-specific miRNA imaging. This dual-logic-gated design reduces off-site signal leakage, enabling robust miRNA imaging with an improved tumor/normal cell discrimination ratio. Furthermore, in vivo studies demonstrate the satisfactory tumor imaging performance of DDN in living mice. Besides, this system is able to distinguish between serum samples from cancer patients and healthy subjects, which underscores its translational potential in clinical diagnosis. This work describes a feasible and powerful logic-gated DNA biosensor for tumor-specific biomarker analysis, showcasing broad application prospects in cancer diagnosis and precision medicine.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"27 1","pages":"182737"},"PeriodicalIF":15.1,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149123228","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}

{"title":"Multifunctional porous polymeric film with radiative cooling and antimicrobial properties for sustainable food preservation","authors":"Zhengxin Ma, Xue Rong, Xueke Wang, Hongbo Zhang, Li Li, Huifang Ma, Jin Yan, Chunmei Ding, Jianshu Li","doi":"10.1016/j.cej.2026.182825","DOIUrl":"https://doi.org/10.1016/j.cej.2026.182825","url":null,"abstract":"Over 30% of global food is lost annually during transit and storage, primarily due to solar irradiation, heat accumulation, and microbial proliferation. Conventional fossil plastic packaging inadequately protects against these threats and exacerbates environmental pollution. Consequently, there is an urgent need for sustainable packaging materials that can simultaneously reflect solar radiation, provide effective cooling under solar irradiation, and inhibit microbial growth. Herein, we report a multifunctional porous packaging film fabricated via a facile single-step casting method using cellulose acetate as the sustainable polymer matrix, with ethylene glycol (EG) as a plasticizer and polyhexamethylene guanidine (PHMG) as an antimicrobial agent. The film spontaneously develops a porous architecture that enables passive radiative cooling, achieving high solar reflectance (>80%) and strong mid-infrared emissivity (>90%) within the atmospheric window. Under solar irradiation, the porous film exhibited average temperature reductions of 17.3 °C, 14.8 °C, and 4.7 °C relative to the reference, CA film, and white paper, respectively, thereby reducing heat accumulation within the packaged food. Concurrently, the incorporation of PHMG endows the film with nearly 100% antibacterial efficacy. Additionally, the film demonstrates exceptional ultraviolet blocking (~100%) and notable antioxidant capabilities. Practical tests confirm the film effectively prevents thermal damage in fresh grapes, inhibits bacterial growth on meat, and delays mushroom browning. By synergizing radiative cooling, antibacterial action, ultraviolet shielding, and antioxidation, this strategy offers a promising pathway for next-generation sustainable food packaging.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"28 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149123167","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}

{"title":"Construction of triazine-based covalent organic framework with enhanced photocatalytic antibacterial performance via imine-linkage isomerization and aqueous-phase synthesis","authors":"Qingqiu Huang, Zhijian Pan, Fang Duan, Fangyuan Zhou, Mengjun Cheng, Shuanglong Lu, Mingliang Du, Jun Wang","doi":"10.1016/j.cej.2026.182727","DOIUrl":"https://doi.org/10.1016/j.cej.2026.182727","url":null,"abstract":"Covalent organic frameworks (COFs) are promising photocatalytic antibacterial materials, yet their performance is often limited by suboptimal photoinduced charge-carrier behavior and weak bacteria–material interfacial interactions under aqueous conditions. Herein, a mild aqueous-phase synthesis strategy was employed to construct triazine-based COFs (Aq-TF-COF) by regulating the imine-linkage orientation. The inversion of the imine linkage altered the local electronic environment, leading to distinct photoinduced charge-carrier characteristics and photocatalytic activities. Meanwhile, compared with the solvothermal route, aqueous-phase synthesis largely retained the characteristic optical properties of the TF-type COF while modifying its surface wettability and facilitating bacteria–material interfacial interactions. Benefiting from the combined effects of favorable photoelectronic and interfacial properties, Aq-TF-COF exhibited the highest photocatalytic antibacterial activity against both <ce:italic>Escherichia coli</ce:italic> (<ce:italic>E. coli</ce:italic>) and <ce:italic>Staphylococcus aureus</ce:italic> (<ce:italic>S. aureus</ce:italic>) among the obtained COFs under identical screening conditions. EPR spectroscopy, fluorescence-probe analyses, and ROS-scavenging experiments supported the involvement of multiple ROS in bacterial inactivation, consistent with the bacterial-envelope damage observed by SEM. These results establish a clear structure-electronics-interface-performance relationship and provide a rational strategy integrating linkage-orientation regulation and aqueous-phase interfacial engineering for the design of efficient COF-based photocatalytic antibacterial materials.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"7 1","pages":"182727"},"PeriodicalIF":15.1,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149123172","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}

{"title":"Gel engineered with nanomaterials for integrated enzymatic reactors (GENIEs) for photothermal real-time PCR","authors":"Sang-A Lee, Minju Park, Hyeongseok Oh, Bong Kyun Kim, Yubeen Hur, Tae Jong Kim, Seuk-Min Ryu, Heesuk Kim, Sang Kyung Kim, Seungwon Jung","doi":"10.1016/j.cej.2026.182685","DOIUrl":"https://doi.org/10.1016/j.cej.2026.182685","url":null,"abstract":"Nanomaterials are frequently employed to enhance in vitro enzymatic reactions, which hold significant importance across diverse bioengineering applications. However, achieving stable dispersion of nanomaterials in these reactions —a prerequisite for practical use—remains an unsolved challenge. Here, we present Gel Engineered with Nanomaterials for Integrated Enzymatic reactors (GENIEs), a hydrogel-based platform designed to physically confine nanomaterials within a porous matrix, thereby ensuring sustained dispersion and functionality throughout the reaction. We incorporated graphene oxide (GO), a widely utilized nanomaterial, into the GENIE framework and generated reduced GO (rGO) -GENIEs via a seamless, in situ chemical reduction step. By leveraging the hydrogel as a structural scaffold, we preserved exceptional dispersity, unlocking the uncompromised photothermal performance of the embedded rGO. The heavily loaded rGO-GENIEs enabled a high-speed photothermal PCR system, achieving rapid heating (13.3 ± 0.7 °C/s) and cooling (11.3 ± 0.4 °C/s) rates via a micro-laser module. Real-time monitoring demonstrated a 95% amplification efficiency and a detection limit of 120 copies/μL for bacterial DNA. These results highlight the potential of the GENIE platform as a robust and versatile reservoir for nanomaterial-integrated assays, enabling superior performance without requiring additional anti-aggregation steps or compromising functionality.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"704 1","pages":"182685"},"PeriodicalIF":15.1,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149123175","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}

{"title":"Co-enabled electron reservoir and in situ catalytic reconstruction on MXene for kinetically enhanced room-temperature Na[sbnd]S batteries","authors":"Chengxing Lu, Boyu Li, Yufei Wang, Yansheng Li, Ziyue Hu, Tianyu Liu, Yuyang Liu, Tong Liu, Ronghui Liu, Baohong Zhang","doi":"10.1016/j.cej.2026.182794","DOIUrl":"https://doi.org/10.1016/j.cej.2026.182794","url":null,"abstract":"Room-temperature sodium‑sulfur (RT Na<ce:glyph name=\"sbnd\"></ce:glyph>S) batteries hold great promise for next-generation energy storage, yet their practical deployment is hindered by the shuttle effect of polysulfides and sluggish reaction kinetics. Herein, an S@Co<ce:inf loc=\"post\">0.5</ce:inf>Ni<ce:inf loc=\"post\">0.5</ce:inf>Se<ce:inf loc=\"post\">2</ce:inf>@MXene composite cathode is designed and an innovative strategy based on in-situ electrochemical reconstruction coupled with synergistic metal displacement is proposed. During cycling, Cu from the current collector dynamically transforms in situ into a highly catalytic Cu<ce:inf loc=\"post\">2</ce:inf>S phase. Concurrently, Co and Ni species from the precursor are displaced and embedded into the electrode matrix as atomically/ionically dispersed species, with Co undergoing reversible valence changes that may contribute to enhanced charge transfer. DFT calculations confirm that the Ni/Co/Se-doped Cu<ce:inf loc=\"post\">2</ce:inf>S exhibits an upshifted d-band center, optimizes polysulfide adsorption, and lowers energy barriers for both the rate-determining step (Na<ce:inf loc=\"post\">2</ce:inf>S<ce:inf loc=\"post\">4</ce:inf> → Na<ce:inf loc=\"post\">2</ce:inf>S<ce:inf loc=\"post\">2</ce:inf>) and Na<ce:inf loc=\"post\">2</ce:inf>S decomposition. This synergistic design enables the cathode to deliver a high capacity of 1441.4 mAh g<ce:sup loc=\"post\">−1</ce:sup> at 5.0 A g<ce:sup loc=\"post\">−1</ce:sup> and remarkable cycling stability, retaining 97.6% of its capacity after 1000 cycles at 2.0 A g<ce:sup loc=\"post\">−1</ce:sup> (0.0024% decay per cycle). This work provides a new paradigm for designing high-performance catalysts via in situ reconstruction for advanced RT Na<ce:glyph name=\"sbnd\"></ce:glyph>S batteries.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"25 1","pages":"182794"},"PeriodicalIF":15.1,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149123232","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}

{"title":"Unlocking cellulose structure disassembly via localized strong adsorption on solid acids for enhanced hydrolysis","authors":"Chengqi Feng, Yuhua Chen, Chenkai Jin, Juncheng Huang, Haining Na, Chao Fang, Jin Zhu","doi":"10.1016/j.cej.2026.182692","DOIUrl":"https://doi.org/10.1016/j.cej.2026.182692","url":null,"abstract":"The effective hydrolysis of cellulose is crucial for valorizing biomass; however, the efficiency of traditional solid acid catalysts is often limited by insufficient adsorption and activation of cellulose. Inspired by the cellulose-binding domain of cellulase, which can disrupt the aggregate structure of cellulose, we used a one-pot hydrothermal method to synthesize carbon-based solid acid catalysts rich in boronic acid hydroxyl (B-OH) and carboxyl (-COOH) groups using furanboronic acid and methylglyoxal as precursors. Catalytic performance evaluation indicates that surface -OH groups (B-OH and C-OH, including phenolic -OH) effectively unlock the aggregate structure of cellulose, significantly improving mass transfer efficiency and thereby promoting cellulose conversion. The optimal catalyst, A1B1@C, achieved a 98.9% cellulose conversion and a 44.7% glucose yield within 4 h in pure water at 180 °C. Mechanistic studies revealed that surface hydroxyl groups, including B-OH and C-OH, collectively disrupt the internal hydrogen-bond network of cellulose through strong adsorption and anchoring. Among them, B-OH is a characteristic and strong binding component. In contrast, the adjacent -COOH groups hydrolyze the exposed glycosidic bonds. Furthermore, the catalyst exhibited excellent cycling stability. This work highlights the critical role of adsorption capacity in solid acid-mediated cellulose conversion and provides a new design strategy for such catalysts.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"11 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149123169","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}

{"title":"Composition-dependent regulation of 2,4,6-trichlorophenol dechlorination by NOM in a PAA/Fe(II) system","authors":"Zhuoyu Li, Zeyu Zhao, Baiyu Yang, Zelin Niu, Chen He, Qianwei Li, Daoqing Liu, Qinghong Wang, Chunmao Chen, Jun Ma","doi":"10.1016/j.cej.2026.182829","DOIUrl":"https://doi.org/10.1016/j.cej.2026.182829","url":null,"abstract":"Natural organic matter (NOM) is commonly regarded as a scavenger of reactive oxygen species (ROS) in advanced oxidation processes, although its redox-active moieties may also promote iron cycling. Here, the composition and concentration-dependent effects of NOM on the degradation and dechlorination of 2,4,6-trichlorophenol (2,4,6-TCP) were investigated in a peracetic acid (PAA)/Fe(II) process. At a concentration of 5 mg C/L, both humic acid (HA) and fulvic acid (FA) elevated 2,4,6-TCP removal within 4 h, and increased chloride release from 171 μM to 213 μM and 254 μM, respectively. However, further increasing the concentration of NOM to 25 mg C/L decreased the removal and dechlorination efficiencies of 2,4,6-TCP in HA based system, whereas FA maintained strong enhancement over a broader concentration range. FA exhibited a much higher electron-donating capacity (3.149 mmol e<ce:sup loc=\"post\">−</ce:sup> gC<ce:sup loc=\"post\">−1</ce:sup>), which was predominantly associated with its high total phenolic content and facilitated Fe(III) reduction and sustained PAA activation. Differently, the phenolic content in HA was lower (1.700 mmol GA gC<ce:sup loc=\"post\">−1</ce:sup>), resulting in the limited Fe(II) restoration but larger scavenging effects under excessive dosages. Besides the typical reactive species of CH<ce:inf loc=\"post\">3</ce:inf>C(O)OO· and Fe(IV) in Fe(II)/PAA system, the addition of NOM increased the contribution of ·OH to the degradation of 2,4,6-TCP. This transformation of reactive species was more pronounced in FA based system. ·OH was generated by the reaction of Fe(II) and organic peroxide radicals (ROO·), which originated from the oxidation of NOM in Fe(II)/PAA system. Molecular characterization further showed that NOM participated in oxidative transformation, accompanied by increased oxygen content and nominal oxidation state of carbon. Real water-derived dissolved organic matter from a natural lake and a biological contact oxidation tank had similar promotion effects on the dechlorination of 2,4,6-TCP, indicating the universality of enhancement of NOM on PAA/Fe(II) system. These results reveal that the important redox mediation of NOM on the stepwise dechlorination in NOM-containing waters.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"21 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149123166","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}

{"title":"Tailored spin-coating strategy for self-assembled monolayer with a specific multifunctional modifier for high-performance inverted perovskite solar cells","authors":"Xiaohuan Zhang, Shan Yuan, Yuxiang Wang, Yuanyuan Zhang, Xiaofei Wei, Qiao Chen, Lili Liu, Wei Yan, Hongyu Chen, Linxing Shi","doi":"10.1016/j.cej.2026.182830","DOIUrl":"https://doi.org/10.1016/j.cej.2026.182830","url":null,"abstract":"The aggregation of self-assembled monolayers (SAMs) and their insufficient surface coverage represent critical bottlenecks in inverted perovskite solar cells (PSCs), elevating carrier extraction barriers and exacerbating non-radiative recombination. In this work, we introduce 4-aminobutyl phosphate hydroiodide (BPAAI) as a multifunctional interfacial modifier and design three distinct spin-coating protocols to identify the optimal configuration for harnessing the multiple interfacial functions of BPAAI. Through combined theoretical calculations and experimental characterizations, the blend spin-coating method is selected as the most effective approach. Systematic investigations reveal that the –PO(OH)<ce:inf loc=\"post\">2</ce:inf> group of BPAAI establishes robust P–O–Ni coordination bonds with NiO<ce:inf loc=\"post\">x</ce:inf>, strengthening interfacial adhesion, while simultaneously coordinating with undercoordinated Pb<ce:sup loc=\"post\">2+</ce:sup> to passivate deep-level defects and suppress non-radiative recombination. Concurrently, the –NH<ce:inf loc=\"post\">3</ce:inf><ce:sup loc=\"post\">+</ce:sup> group forms hydrogen bonds with FA<ce:sup loc=\"post\">+</ce:sup>, inhibiting the formation of FA<ce:sup loc=\"post\">+</ce:sup> vacancies and directing preferential crystal orientation growth. More importantly, local charge-dipole interactions between the –NH<ce:inf loc=\"post\">3</ce:inf><ce:sup loc=\"post\">+</ce:sup> groups and SAM molecules together with the steric hindrance of BPAAI effectively mitigate molecular aggregation, thereby improving film uniformity, optimizing energy-level alignment, and boosting charge-carrier extraction and transport. Consequently, the BPAAI-modified PSCs deliver a champion power conversion efficiency of 26.52%, accompanied by markedly enhanced operational stability, and the unencapsulated device retains approximately 90% of its initial efficiency after roughly 1000 h of continuous maximum power point tracking. This work establishes a universal spin-coating strategy for buried-interface engineering, effectively resolving SAM-related challenges and advancing stable, high-efficiency inverted PSCs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"9 1","pages":"182830"},"PeriodicalIF":15.1,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152274","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}

{"title":"Physics-informed LSTM for lignocellulosic pyrolysis kinetics at elevated heating rates: Integrating Arrhenius constraints with data-driven modeling","authors":"Yuanbo Song, Mengyu Jin, Xintong Meng, Yalei Zhang, Kai Zhang, Zheng Shen","doi":"10.1016/j.cej.2026.182266","DOIUrl":"https://doi.org/10.1016/j.cej.2026.182266","url":null,"abstract":"Reliable prediction of lignocellulosic intermediate pyrolysis kinetics is critical for scaling up thermochemical conversion processes, yet remains challenging at high heating rates. We developed a physics-informed long short-term memory network (PINN-LSTM) integrating particle swarm optimization (PSO) with recurrent neural networks, trained on only 13 thermogravimetric/derivative thermogravimetric (TG/DTG) curves from pure components, blends, and real straws. PSO inversely determines apparent phenomenological kinetic triplets (<mml:math altimg=\"si1.svg\" display=\"inline\"><mml:mi>E</mml:mi></mml:math>, <mml:math altimg=\"si5.svg\" display=\"inline\"><mml:mi>A</mml:mi></mml:math>, <mml:math altimg=\"si6.svg\" display=\"inline\"><mml:mi>n</mml:mi></mml:math>), embedded as Arrhenius-based soft constraints in the LSTM loss function, enforcing physical feasibility without compromising flexibility. On the three held-out straws PINN-LSTM attains RMSE values of 0.80, 0.78 and 0.80 wt%·min<ce:sup loc=\"post\">−1</ce:sup>, corresponding to a 43% reduction in mean RMSE relative to the vanilla LSTM and approximately 76% relative to HRF, the strongest tree ensemble; each comparison is stated against a single named baseline rather than as a combined range. The model accurately captures shoulder-peak transitions and high-temperature tails, with peak-temperature errors below 1 K. The <ce:italic>E</ce:italic>-ln<ce:italic>A</ce:italic> relationship observed is that expected under single-heating-rate inversion and is reported as an apparent, jointly determined descriptor rather than as an independently established physical law. A web-based interface enables real-time parameter estimation (<mml:math altimg=\"si7.svg\" display=\"inline\"><mml:mi>E</mml:mi><mml:mo>=</mml:mo><mml:mn>228</mml:mn></mml:math> kJ·mol<ce:sup loc=\"post\">−1</ce:sup>, <mml:math altimg=\"si8.svg\" display=\"inline\"><mml:mi>ln</mml:mi><mml:mi>A</mml:mi><mml:mo>=</mml:mo><mml:mn>42.1</mml:mn></mml:math> s<ce:sup loc=\"post\">−1</ce:sup>, <mml:math altimg=\"si9.svg\" display=\"inline\"><mml:mi>n</mml:mi><mml:mo>=</mml:mo><mml:mn>2.31</mml:mn></mml:math>) with automated visualization, facilitating industrial adoption. This synergy between data-driven learning and physics-based constraints demonstrates broader applicability to thermochemical systems with mechanistic priors and data scarcity.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"28 1","pages":"182266"},"PeriodicalIF":15.1,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149123173","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}

{"title":"Atom-to-reactor engineering of 3D-printed Ni-N/SiOC monolithic catalysts with interfacial dual-site synergy for robust low-temperature CO2 methanation","authors":"Honglei Mi, Xiaoyue Guo, Yifan Zhang, Zuojiang You, Yaohan Kong, Jianqi Yao, Dong Zhang, Mei Gu, Fang Qian, Faliang Luo","doi":"10.1016/j.cej.2026.182745","DOIUrl":"https://doi.org/10.1016/j.cej.2026.182745","url":null,"abstract":"CO<ce:inf loc=\"post\">2</ce:inf> methanation is a key technology for renewable energy grid integration, yet its practical implementation is hindered by the kinetic bottleneck of low-temperature CO<ce:inf loc=\"post\">2</ce:inf> activation and the persistent disconnect between atomic-level active-site optimization and macroscale reactor design. Herein, we proposed an “atom-to-reactor” synergistic engineering strategy and demonstrated it through a one-pot, additive-free Direct Ink Writing (DIW) 3D printing approach to fabricate N-regulated Ni-N/SiOC monolithic catalysts. This strategy simultaneously achieved atomic-level electronic reconfiguration of Ni active sites via N-doping and macroscale construction of a hierarchical pore network via 3D printing. N doping formed stable Ni-N<ce:inf loc=\"post\">X</ce:inf> coordination structures that induced continuous electron transfer from N to Ni. This yielded electron-enriched Ni<ce:sup loc=\"post\">0</ce:sup> sites and created an “interfacial dual-site” effect, where N-anchored strong basic sites and adjacent Ni<ce:sup loc=\"post\">0</ce:sup> sites synergistically couple CO<ce:inf loc=\"post\">2</ce:inf> adsorption with H<ce:inf loc=\"post\">2</ce:inf> activation. The 3D-printed monolithic architecture integrated interconnected macropores with micro/mesoporous struts, ensuring efficient mass transfer and full exposure of active sites. The Ni<ce:glyph name=\"sbnd\"></ce:glyph>N coordination further served as a strong anchoring site, inhibiting Ni particle sintering during 130 h operation and preserving the integrity of the hierarchical diffusion network. The optimal 15% Ni-N/SiOC monolithic catalyst delivered 97.79% CO<ce:inf loc=\"post\">2</ce:inf> conversion and 100% CH<ce:inf loc=\"post\">4</ce:inf> selectivity at 320 °C, and retained 86.43% conversion at the low temperature of 260 °C, with an activity decay rate below 7% over 130 h. A direct comparison between monolithic and powdered forms confirmed the indispensability of the 3D-printed architecture for fully realizing the intrinsic activity. In-situ DRIFTS revealed a formate-CO dual-path synergism, wherein the two pathways complement each other across different temperature windows, effectively overcoming the low-temperature kinetic limitation.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"78 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149123233","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}