Chen Chen, Xinlu Li, Weixia Zhu, Yu Chen, Jie Tang, Shun Yao
{"title":"The suppository containing a complex of active pharmaceutical ingredient-ionic liquid (API-IL) derived from mefloquine and artesunate with Zeolitic imidazolate framework-8","authors":"Chen Chen, Xinlu Li, Weixia Zhu, Yu Chen, Jie Tang, Shun Yao","doi":"10.1016/j.cej.2025.169534","DOIUrl":"https://doi.org/10.1016/j.cej.2025.169534","url":null,"abstract":"This study aimed to develop a new suppository containing the complex of active pharmaceutical ingredient-ionic liquid (API-IL) and metal organic framework. As two famous drugs with anti-virus activities for the combination therapy of COVID-19, mefloquine (MQ) hydrochloride and artesunate (Art) were combined and then transformed to API-ILs to enhance therapeutic effects. The synthesized [MQ][Art] was characterized using melting point tests, Fourier transform infrared spectrum (FT-IR), proton nuclear magnetic resonance (<sup>1</sup>H NMR), and mass spectroscopy (MS). Furthermore, [MQ][Art] exhibited improved water solubility, stability and pH values, which promoted treatment effectiveness while minimizing intestinal irritation during administration. Subsequently, [MQ][Art] was incorporated into Zeolitic imidazolate framework-8 (ZIF-8) to further enhance stability and achieve a controlled release effect. Combined with computational studies on interactive energy between ZIF-8 and API-IL, comprehensive characterizations confirmed the successful incorporation of [MQ][Art] on ZIF-8. The preparation method of suppositories was then investigated; among the 9 tested suppository bases, poloxamer-based suppositories demonstrated uniform quality with suitable hardness and melting time while also exhibiting a controlled release effect on [MQ][Art]. After 10 h of cumulative release rate testing reached 90 %. Finally, the poloxamer-based suppository containing [MQ][Art]@ZIF-8 showed good quality uniformity with an average drug content of 11.4 mg per suppository and an average displacement value of 2.59. Besides that, the in vivo release process was detected to demonstrate the effectiveness of the developed system. In conclusion, the combination of API-ILs with ZIF-8 in suppositories designed for COVID-19 treatment enhances therapy effectiveness by improving solubility and stability while also providing controlled release effects on MQ and Art.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"34 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145261105","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":"Microfluidic device for high-throughput cancer drug screenings","authors":"Po-Hsun Chen, Lin-Yu Wang, Chia-Yuan Chang, Yuh-Shiuan Chien, Yu-Chia Su, Chi-Kuang Wang, Kuang-Chong Wu, Hsian-Jean Chin, Chien-Fu Chen","doi":"10.1016/j.cej.2025.169510","DOIUrl":"https://doi.org/10.1016/j.cej.2025.169510","url":null,"abstract":"High-throughput drug screening is critical in discovering therapeutic compounds, but traditional manual dilution methods are laborious, error-prone, and inefficient. Here, we report on the development of a microfluidic device designed to generate drug concentration gradients accurately and rapidly. This device utilizes laminar flow at low Reynolds numbers to precisely control the volume ratio of the two mixed fluids by adjusting channel length, helping to create precise dilution ratios from 1/3× to 1/300×. We demonstrated that the resulting concentration gradient deviated less than 6 % from the target value, significantly better than manual dilution methods, using bovine serum albumin (BSA) as a sample to simulate actual drug dilution. Furthermore, the device was validated through cytotoxicity tests of the dilution of chemotherapy drug (oxaliplatin) on colorectal cancer cells (HCT-116). The IC<sub>50</sub> deviation obtained from the microfluidic device was within 2.45 % of those obtained by manual dilution, showcasing its reliability and accuracy. Multi-drug screening involving 5-FU, oxaliplatin and SN-38 on HCT-116 cells was also conducted to demonstrate the device's applicability in complex screening. Notably, the device achieves steady-state within 30 s at high flow rates, demonstrating scalability and potential for integration into high-throughput screening platforms. This technology reduces the time and labor required for drug screening and improves dilution accuracy, providing a promising avenue for personalized and precision medicine.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"18 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145261106","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}
Jiujiu Tian, Xiaojiang Mu, Yitong Wang, Hailan Zhao, Lu Yin, Fan Zhang, Xiaoyang Wang, Lei Miao
{"title":"Hierarchical solar interface evaporator derived from natural multilevel plant leaves for high-efficiency desalination","authors":"Jiujiu Tian, Xiaojiang Mu, Yitong Wang, Hailan Zhao, Lu Yin, Fan Zhang, Xiaoyang Wang, Lei Miao","doi":"10.1016/j.cej.2025.169468","DOIUrl":"https://doi.org/10.1016/j.cej.2025.169468","url":null,"abstract":"Solar-driven interfacial evaporation has emerged as a sustainable strategy for seawater desalination. However, achieving both high energy utilization and ultrafast evaporation under standard solar illumination remains challenging. In this work, we present a hierarchical solar interface evaporator derived from carbonized natural plant leaves, which retain intrinsic multilevel architectures including vascular channels, surface micro-textures, and interlayer porosity. These structures facilitate efficient water transport, broad-spectrum light absorption, and rapid vapor escape. More importantly, the hierarchical system enables multistage energy utilization by coupling direct solar absorption with passive environmental energy harvesting and latent heat recycling from upper to lower evaporation stages. As a result, the 9-stage evaporator attains an exceptionally high evaporation rate of 6.12 kg m<sup>−2</sup> h<sup>−1</sup> for 1 h under 1-sun (1 kW m<sup>−2</sup>) without external energy input, significantly surpassing the thermodynamic limit of conventional single-stage systems. The system also exhibits excellent long-term stability and salt rejection in continuous desalination tests. This study demonstrates the feasibility of using carbonized natural materials to construct low-cost, high-efficiency evaporators and offers new insights into multistage energy utilization strategies for practical water purification applications.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"89 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145255003","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}
Tinghui Deng, Bai Wang, Dongshu Chen, Siyu Han, Jie Ren, Shujun Liu, Jianshe Hu
{"title":"Deep learning-enhanced wear-resistant antimicrobial polyurea-based ionogels for real-time firefighter motion tracking in extreme environments","authors":"Tinghui Deng, Bai Wang, Dongshu Chen, Siyu Han, Jie Ren, Shujun Liu, Jianshe Hu","doi":"10.1016/j.cej.2025.169444","DOIUrl":"https://doi.org/10.1016/j.cej.2025.169444","url":null,"abstract":"Flexible sensors are critical for monitoring the vital signs of firefighters but face substantial challenges in urgent scenarios (e.g., emergency rescues), including mechanical damage, biofouling, and high-temperature instability. To address these issues, we developed a polyurea-based ionogel (Pub-xIL) via a catalyst-free ambient synthesis strategy, in which ionic liquids are incorporated into polyurea matrices. By tuning molecular ratios (PPG2000/PPG400 and MDI/HMDI), hierarchical H-bond networks were engineered, endowing Pub-xIL with exceptional mechanical properties: tensile strength of 1.7 MPa, puncture resistance (6.95 N load capacity), tear resistance (fracture energy = 2989 J/m<sup>2</sup>), and self-healing properties. Standardized quantitative wear resistance analysis showed that Pub-xIL had a wear index of 0.046 mg/cycle, outperforming traditional flexible sensor substrates such as polydimethylsiloxane, polyimide, and polyethylene terephthalate. Additionally, Pub-xIL maintained stable performance across a broad temperature range (−20 to 60 °C). The functional ionic liquid [EMIM][TFSI] confers dual advantages on Pub-xIL: it achieves >99 % inhibition rates against <em>Staphylococcus aureus</em> and <em>Escherichia coli</em> and yields a high strain coefficient (GF = 3.79, enabling precise motion detection). Integrating the Pub-xIL sensor array with machine learning algorithms enabled real-time classification of dynamic movements (e.g., walking, running) and static postures (e.g., standing, lying down) with a classification accuracy over 96 %. This work enhances situational awareness and survival prospects in life-critical rescue missions, while establishing a pioneering platform for next-generation firefighting wearable systems.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"24 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145255067","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}
Han Cheng, Yanbing Pan, Tao Fang, Uchkun Ishimov, Awais Ihsan, Abrar Hussain, Ruiting Tian, Wenwen Ma, Jun Li, Xianju Huang
{"title":"Preparation of AuSe-BNPs/CFME and its high-sensitivity simultaneous detection of caffeic acid and dihydrotanshinone I","authors":"Han Cheng, Yanbing Pan, Tao Fang, Uchkun Ishimov, Awais Ihsan, Abrar Hussain, Ruiting Tian, Wenwen Ma, Jun Li, Xianju Huang","doi":"10.1016/j.cej.2025.169449","DOIUrl":"https://doi.org/10.1016/j.cej.2025.169449","url":null,"abstract":"Caffeic acid (CA) and dihydrotanshinone I (DHT I) are two important natural products that have become a research hotspot because of their significant antioxidant, anti-inflammatory, and anti-tumour fields. Bimetallic gold‑selenium nanoparticles (AuSe-BNPs) were prepared using the water-bath reduction method, and a carbon fiber microelectrode modified by AuSe BNPs composites (AuSe-BNPs/CFME) was constructed for the detection of CA and DHT I. The electrochemical performance of the AuSe-BNPs/CFME was characterised by using cyclic voltammetry (CV), differential pulse voltammetry (DPV) and electrochemical impedance spectroscopy (EIS). The good electrical conductivity of AuSe BNPs/CFME was confirmed. CA concentration in the range of 1.0–10.0 μmol/L and DHT I concentration in the range of 0.1–1.0 μmol/L showed a good linear relationship with the oxidation peak currents, and the limits of detection (LODs) of 0.88 μmol/L and 0.0055 μmol/L, respectively. The modified electrode exhibited good anti-interference properties when coexisting with common ions or relevant active ingredients. It was applied to the determination of CA and DHT I in human serum, with recovery rates ranging from 99.1 % to 104.3 %, and can be used for the detection of actual samples.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"89 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145255070","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":"Smart paper-based sensor: A novel bio-enzyme-free dual-mode platform for real-time visual monitoring of organophosphorus pesticides","authors":"Wanqi Jiang, Chuang Jiang, Xiyao Liang, Shuqing Mei, Yuqing Zhang, Yingying Feng, Yaqing Xiao, Yingnan Liu","doi":"10.1016/j.cej.2025.169503","DOIUrl":"https://doi.org/10.1016/j.cej.2025.169503","url":null,"abstract":"This study proposed a colorimetric/fluorescent bimodal bio-enzyme-free paper-based sensor for device-free visual detection of organophosphorus (OPs). The Zn-doped Fe-based organic framework (MIL-88B-Fe/Zn) exhibited excellent peroxide-like activity, catalyzing the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H<sub>2</sub>O<sub>2</sub>. The oxidized TMB displayed blue color and quenched the red fluorescence of carbon dots derived from neutral red (NR-CDs) through inner filter effect (IFE). In the presence of OPs, the enzyme-like activity of MIL-88B-Fe/Zn was inhibited due to the collapse of MOF structure, which hindered the chromogenic reaction of TMB, while the fluorescence of NR-CDs was restored by IFE deactivation. TMB and NR-CDs were co-modified on filter paper to construct T-N paper with dual signal responses. As OPs concentration increased, T-N paper changed from blue to red under daylight, and red fluorescence enhanced under UV light. Photographs were captured by smartphone, and standard curves of OPs concentration versus R/B values (colorimetric) and R values (fluorescent) were established for quantitative analysis. Detection limits for glyphosate were 1.04 ng/mL (colorimetric) and 1.22 ng/mL (fluorescent). This sensor was simple to operate, multi-signal self-calibrated, and highly portable, providing a new strategy for rapid on-site detection of OPs residues and the construction of bio-enzyme-free trace analysis platform.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"204 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145255112","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}
Ji Ding, Ao-Ping Wu, Huihui Zhang, Huiying Liao, Pengfei An, Sheng Dai, Zhi-Qiang Wang, Zhenshan Hou
{"title":"Alkali halides induced electron-deficient oxygen vacancies on polyoxometalates promoting CO2 hydrogenation","authors":"Ji Ding, Ao-Ping Wu, Huihui Zhang, Huiying Liao, Pengfei An, Sheng Dai, Zhi-Qiang Wang, Zhenshan Hou","doi":"10.1016/j.cej.2025.169472","DOIUrl":"https://doi.org/10.1016/j.cej.2025.169472","url":null,"abstract":"The development of catalysts for the efficient catalytic conversion of CO<sub>2</sub> remains a significant challenge. Herein, a series of alkali halide-modified polyoxometalate (POM) catalysts with substituted Ru single atoms were constructed for efficient CO<sub>2</sub> hydrogenation. Characterization using XRD, ESI-MS, in-situ FT-IR, HAADF-STEM and XAFS confirmed that the single-atom Ru were incorporated into the POM framework. Notably, the introduction of LiCl modulating electron-deficient oxygen vacancies (O<sub>V</sub>) on the POM surface can effectively promote the dissociation of H<sub>2</sub>. Moreover, the single-atom Ru facilitated the adsorption of CO<sub>2</sub> and formed the bidentate carbonate intermediate (b-CO<sub>3</sub>). Then, the reactive hydrogen species on the O<sub>V</sub> sites enhanced the selective hydrogenation of CO<sub>2</sub> to CO, thereby promoting the reverse water gas shift (RWGS) reaction. In-situ RWGS reaction FT-IR and DFT calculations jointly revealed the synergistic effect of electron-deficient O<sub>V</sub> and single-atom Ru on promoting H<sub>2</sub> dissociation and CO<sub>2</sub> adsorption. In addition, the CO produced from the RWGS reaction can be subsequently utilized in the hydroformylation of olefins using a conventional catalytic system consisting of rhodium complex and phosphine ligands, thereby achieving the conversion of CO<sub>2</sub> into valuable chemicals.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"89 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145255120","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}
Dan Han, Lianao Yan, Yu Wang, Yuru Pang, Zhekai Zhang, Xiuli He, Guojing Wang, Weidong Wang, Shengbo Sang
{"title":"Highly conductive GaN-Cu3(HITP)2/PANI gas sensor based on GaN double heterojunction coupled with deep learning for accurate trimethylamine mixed gas detection","authors":"Dan Han, Lianao Yan, Yu Wang, Yuru Pang, Zhekai Zhang, Xiuli He, Guojing Wang, Weidong Wang, Shengbo Sang","doi":"10.1016/j.cej.2025.169488","DOIUrl":"https://doi.org/10.1016/j.cej.2025.169488","url":null,"abstract":"Metal-Organic Frameworks (MOFs) have attracted extensive attention in the field of gas sensing. However, single MOFs materials suffer from shortcomings such as poor electrical conductivity and easy agglomeration, leading to limited performance. Herein, the highly conductive GaN-M<sub>3</sub>(HITP)<sub>2</sub>/PANI nanocomposites were synthesized through in-situ method on GaN-HP film. Due to the higher degree of protonation caused by hierarchically porous architecture, the GaN-Cu<sub>3</sub>(HITP)<sub>2</sub>/PANI sensor demonstrates better TMA sensing performance compared with GaN-Ni<sub>3</sub>(HITP)<sub>2</sub>/PANI sensor. The GaN-Cu<sub>3</sub>(HITP)<sub>2</sub>/PANI sensor achieves a lower detection limit of 500 ppb, higher response value for 100 ppm TMA (91.4 %), faster response/recovery rate (21 s/56 s) at room temperature. Moreover, the GaN-Cu<sub>3</sub>(HITP)<sub>2</sub>/PANI sensor exhibits good long-term stability and humidity resistance. Systematic analysis revealed that the enhanced sensing performance in the GaN-Cu<sub>3</sub>(HITP)<sub>2</sub>/PANI composite stems from the formation of coupled heterointerface system and its hierarchically porous architecture. The Douglas-Peucker (DP) algorithm was used for the first time to extract the response features of GaN-Cu<sub>3</sub>(HITP)<sub>2</sub>/PANI sensor, and combined with a deep learning algorithm, successfully achieving exact recognition of the mixed gas of TMA and MH<sub>3</sub>, with an identification rate as high as 94.1 %.Thus, the GaN-Cu<sub>3</sub>(HITP)<sub>2</sub>/PANI sensor provides a feasible solution for developing portable TMA detection systems embedded into smart wearable devices.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"20 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145261059","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}
Minjun Je, Jihun Sung, Jihoon Oh, Heejin Kim, Dongmin Park, Hyoyeong Kim, Youngjin Song, Sang-Min Lee, Jang Wook Choi, Soojin Park
{"title":"Polysulfide-mediated solid-state wetting for low-pressure all-solid-state lithium metal batteries","authors":"Minjun Je, Jihun Sung, Jihoon Oh, Heejin Kim, Dongmin Park, Hyoyeong Kim, Youngjin Song, Sang-Min Lee, Jang Wook Choi, Soojin Park","doi":"10.1016/j.cej.2025.169406","DOIUrl":"https://doi.org/10.1016/j.cej.2025.169406","url":null,"abstract":"The quest for practical all-solid-state lithium metal batteries (ASSLMBs) has focused on achieving reliable operation at room temperature and low stack pressure. However, attempts to lower this pressure have proved challenging due to interfacial instabilities and unwanted lithium (Li) dendritic growth. Here, we introduce a solid-state wetting approach of the Li metal anode by utilizing a polysulfide derived from α-lipoic acid (LA) and lithiophilic tin (Sn) seeds. The polymeric network constructs strong interfacial bridges between the Li metal and solid electrolyte, while simultaneously driving the depth-wise redistribution of the pulverized Sn seeds throughout the bulk Li metal, thereby achieving comprehensive solid-state wetting that extends across the anode structure. This architecture, by concurrently mitigating the interfacial and bulk instabilities in Li<sub>0.97</sub>Mg<sub>0.03</sub> metal anodes, enables stable operation at room temperature and low stack pressure (2.5 MPa), along with exceptional capacity retention of 86.7 % over 160 cycles at 0.5C with a high areal capacity of 3.5 mAh cm<sup>−2</sup>. This study establishes foundational guidelines for the design of Li metal anodes toward high-performance ASSLMBs under practical operating conditions.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"122 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145261060","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":"Interaction between neighboring sulfur vacancies facilitates highly efficient nitrogen fixation in single-layer FeNiP2S6-x","authors":"Ka Wang, Hengdong Ren, Ruilin Guan, Zhichao Wang, Yuxiang Yan, Wenqing Wei, Haizeng Song, Lei Feng, Siying Ma, Zijing Guo, Qingkai Tang, Xianghong Niu, Shancheng Yan, Xinglong Wu","doi":"10.1016/j.cej.2025.169532","DOIUrl":"https://doi.org/10.1016/j.cej.2025.169532","url":null,"abstract":"Iron-based transition metals, particularly iron-based thiophosphates, have attracted significant interest due to their ability to regulate iron electronic states through surface defect engineering. In this work, we fabricated and subsequently exfoliated single-layer FeNiP<sub>2</sub>S<sub>6-x</sub> (SL-FeNiP<sub>2</sub>S<sub>6-x</sub>), where mild and selective B(OH)<sub>3</sub> etching generated a disordered distribution of surface sulfur vacancies (SVs) for efficient nitrogen reduction reactions (NRR). Single-layer theoretical calculations suggest that interactions between neighboring SVs significantly enhance nitrogen fixation, with single-double sulfur vacancy (S-DSV) interactions causing the most pronounced shift in the d-band center of iron atoms towards the Fermi level. The improved alignment between the production rates of *NN and *H indicates that S-DSV enhances the catalytic activity of FeNiP<sub>2</sub>S<sub>6-x</sub> more effectively than single-single sulfur vacancy (S-SSV) or double-double sulfur vacancy (D-DSV), and far outperforms isolated SSV or DSV. Electrochemical tests demonstrated that in a 0.1 M KOH solution at −0.1 V, SL-FeNiP<sub>2</sub>S<sub>6-x</sub> with a sufficient concentration (>50 %) of S-DSV achieved a Faraday efficiency (FE) of 51.30 % and an NH<sub>3</sub> yield of 96.52 μg h<sup>−1</sup> mg<sup>−1</sup>, surpassing the performance of previously reported NRR catalysts. This work introduces a useful strategy for enhancing electrocatalytic activity by strategically manipulating the position and distribution of adjacent non-metal atom vacancies on the surface.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"53 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145261067","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}