Journal of Colloid and Interface Science最新文献

{"title":"Core-shell structure-induced exciton unidirectional transport in PhC2Cu for enhanced antibiotics degradation","authors":"Yishun Wang,&nbsp;Yufeng Zeng,&nbsp;Zili Lin,&nbsp;Xiaoyu Zhang,&nbsp;Yu Chen,&nbsp;Ping Chen,&nbsp;Wenying Lv,&nbsp;Guoguang Liu","doi":"10.1016/j.jcis.2025.137915","DOIUrl":"10.1016/j.jcis.2025.137915","url":null,"abstract":"<div><div>For this work, a novel heterogeneous PhC₂Cu/ZnO, function of facilitating unidirectional exciton transport, was successfully constructed. Leveraging ZnO’s robust electron transfer capability, highly efficient delocalization of photogenerated electrons, and rapid separation of photogenerated carriers from PhC₂Cu was achieved, leading to improved photocatalytic performance. Remarkably, the addition of just 5 % ZnO enhanced the photocatalytic degradation ability of ciprofloxacin (CIP) by 4.24 times (15 min, 95.2 %). In addition, the issues related to the wide bandgap and photocorrosion of ZnO were effectively circumvented through our designed strategy. Meanwhile, the electron delocalization effect within PhC₂Cu enhances its molecular stability, which in turn improves the photocatalyst’s performance and long-term recyclability. Moreover, the impact of different ZnO morphologies on exciton transport was systematically investigated, with the core–shell structure identified as most conducive to efficient interface electron transfer. Through in-situ XPS analysis, the exciton unidirectional transport effect was directly demonstrated.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"696 ","pages":"Article 137915"},"PeriodicalIF":9.4,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144089894","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"The role of iron in Ni-Fe binary catalysts for electrochemical glycerol oxidation","authors":"Yanming Li,&nbsp;Honglei Chen,&nbsp;Feng Gao,&nbsp;Qi Chen,&nbsp;Changli Li,&nbsp;Jingfu He","doi":"10.1016/j.jcis.2025.137913","DOIUrl":"10.1016/j.jcis.2025.137913","url":null,"abstract":"<div><div>NiFe binary compounds have shown great potential in the electrocatalytic oxidation of biomass-derived glycerol towards valuable products. However, understanding the role of Fe on the glycerol oxidation process of Ni-based catalysts remains challenging due to the complex multi-alcohol-group oxidation. Herein, our systematic study identifies that Fe can improve both the dynamic process of Ni(OH)₂ transformation into active NiOOH and the kinetic process of redox reaction between NiOOH and glycerol. Specifically, the introduction of Fe can significantly reduce the onset potential of glycerol oxidation by &gt; 100 mV while maintaining &gt; 95 % selectivity of HCOOH. The in situ Raman results show that the Ni²⁺/Ni³⁺ conversion potential is exactly the same as the onset potential of glycerol oxidation, indicating that NiOOH is the most important active structure, and Fe doping can optimize the dynamic process of NiOOH generation. The electrochemical dynamic analysis reveals that the oxidation of glycerol on Ni-based catalysts follows an electrochemical-chemical process, and the chemical reaction constant (<em>k</em>) value is greatly improved by 5 times with the presence of Fe. Density functional theory (DFT) calculation reveals that the electron transfer from Fe to Ni can help the extraction of electrons from adsorbed glycerol, thus lowering the reaction barrier and accelerating the reaction rate. Based on this, we constructed an efficient photoanode with Metal-Insulator-Semiconductor (MIS) junction structure (<em>n</em>-Si/SiO<em>_x</em>/Ni₃Fe₁) that demonstrated the highest glycerol oxidation photocurrent and excellent selectivity for formate.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"697 ","pages":"Article 137913"},"PeriodicalIF":9.4,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144108059","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Engineering the interface charge redistribution and boosted kinetics via polyoxometalate for efficient carbon dioxide electroreduction in acidic medium","authors":"Wencong Sun ,&nbsp;Chunxiang Li ,&nbsp;Li Zhou ,&nbsp;Wenxue Tian ,&nbsp;Shumiao Li ,&nbsp;Min Yang","doi":"10.1016/j.jcis.2025.137912","DOIUrl":"10.1016/j.jcis.2025.137912","url":null,"abstract":"<div><div>The development of electrocatalytic CO₂ reduction reaction (ECO₂RR) which can achieve carbon neutrality goals in acidic medium can effectively solve the problems of carbonate formation and low CO₂ utilization efficiency, but the inhibition of hydrogen evolution reaction (HER) is challenging. Thus, a co-modification strategy of electrolyte and electrocatalyst has been proposed to solve this issue. In a polyoxometalate (POM) H₆PV₃Mo₉O₄₀ modified acidic medium, the highest Faradaic efficiency (FE) and current density for carbonaceous product of POM-CuSe/rGO reach 90.8% and −176.2 mA·cm⁻², respectively. Detailed research shows that the modification for catalyst by POM results in a redistribution of interfacial charges which favors the stable adsorption of *CO, as well as a reduction in the lateral size from 42 ∼ 1400 to 27 ∼ 167 nm. While the POM modification of the electrolyte leads to enhanced kinetics and suppressed CO₃²⁻ production, achieving a single pass conversion efficiency for CO of up to 69.0%. This work proposes a new strategy of POM co-modification for electrolyte and electrocatalyst to enhance the efficiency of acidic CO₂ conversion for industrial applications.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"697 ","pages":"Article 137912"},"PeriodicalIF":9.4,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144134279","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Polypyrrole-decorated Vulcan XC-72R support enables a low platinum content PtRu catalyst toward alkaline hydrogen oxidation reaction","authors":"Xingyan Chen ,&nbsp;Dingge Fan ,&nbsp;Xi Lin ,&nbsp;Siyan Chen ,&nbsp;Jiahe Yang ,&nbsp;Pin Meng ,&nbsp;Hongda Shi ,&nbsp;Wei Zheng ,&nbsp;Yunlong Zhang ,&nbsp;Yang Yang ,&nbsp;Dongdong Wang ,&nbsp;Qianwang Chen","doi":"10.1016/j.jcis.2025.137908","DOIUrl":"10.1016/j.jcis.2025.137908","url":null,"abstract":"<div><div>PtRu alloys are promising catalysts for the hydrogen oxidation reaction (HOR) in alkaline hydroxide exchange membrane fuel cells (HEMFCs) for commercial application. However, there is a need to lower the loading of platinum while simultaneously increasing its activity. Herein, we successfully prepared a PtRu alloy catalyst featuring a precisely controlled Pt-to-Ru atomic ratio of 1:5, which is typically 1:1 or 1:3, supported on polypyrrole (Ppy) decorated Vulcan XC-72R (XC). The catalyst, named Pt₁Ru₅/Ppy-XC, exhibits a remarkable mass catalytic activity of 10.69 ± 1.40 mA μg_PGM⁻¹, which is 7.2-fold and 2.6-fold higher than those of commercial PtRu/C and Pt₁Ru₅ nanoparticles supported on raw XC, respectively. Moreover, the HEMFC with Pt₁Ru₅/Ppy-XC anode achieves a peak power density of 1.53 W cm⁻² (0.15 mg_PGM cm_anode⁻²), outperforming that of Pt₁Ru₅/XC (1.26 W cm⁻², 0.18 mg_PGM cm_anode⁻²). The combined experimental characterization and theoretical calculations reveal that Ppy significantly enhances the active site density due to the decrease in the proportion of micropores while optimizing the binding strength of *H and *OH species on Pt₁Ru₅/Ppy-XC, resulting in excellent catalytic performance even with a low Pt usage. This work provides a novel strategy for developing high-performance electrocatalysts by employing functionalized XC support to fine-tune catalyst/support interactions and control over the pore structure of carbon supports.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"697 ","pages":"Article 137908"},"PeriodicalIF":9.4,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144108061","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synthesis of heteroatom zeolite subcrystals as catalytic materials and structural building blocks","authors":"Ke Du,&nbsp;Jiayu Yu,&nbsp;Pingping Wang,&nbsp;Di Pan,&nbsp;Zhaoqi Ye,&nbsp;Wanyi Li,&nbsp;Ling Ding,&nbsp;Wei Chen,&nbsp;Yi Tang,&nbsp;Yahong Zhang","doi":"10.1016/j.jcis.2025.137909","DOIUrl":"10.1016/j.jcis.2025.137909","url":null,"abstract":"<div><div>Recent advancements in zeolite synthesis techniques have facilitated the synthesis of heteroatom zeolites with customized acidity and redox properties. However, challenges remain in controlling the content, accessibility and distribution of active center. A new zeolite construction strategy is still desired for the design of effective heteroatom zeolite catalysts. In this work, we synthesized and extracted a series of highly short-range ordered heteroatom-containing MFI zeolite subcrystals (Al, Ga, Ti, Zn, and Sn) with open framework structures and tunable acidic properties. These heteroatom-containing zeolite subcrystals not only acted as catalyst materials with diverse catalytic activity and high active site accessibility, but also served as versatile building blocks for customized zeolite synthesis and active site modulation via non-classical aggregation and cross-aggregation crystallization processes. Notably, we demonstrated that the catalytic performance of the unique subcrystals and their aggregated products were tailored to meet the specific requirements of reactions such as olefin epoxidation and macromolecular cracking. Furthermore, this synthesis strategy was also applicable to the synthesis of MEL zeolite subcrystals. The continuous expansion of subcrystal category opens new avenues for the design of multifunctional zeolite catalysts, contributing valuable insights into zeolite synthesis and active site regulation.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"697 ","pages":"Article 137909"},"PeriodicalIF":9.4,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088766","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Alumina-supported palladium modified by zeolite Socony Mobil-5 for highly efficient selective hydrogenation of acetylene in excess ethylene","authors":"Huiran Zhou ,&nbsp;Bohui Ye ,&nbsp;Huigen Fu ,&nbsp;Xiaolong Wei ,&nbsp;Zhongke Ma ,&nbsp;Haonan Yin ,&nbsp;Yangyang Yuan ,&nbsp;Yang Liu","doi":"10.1016/j.jcis.2025.137907","DOIUrl":"10.1016/j.jcis.2025.137907","url":null,"abstract":"<div><div>Catalytic selective hydrogenation of acetylene plays an indispensable role during polymer-grade ethylene manufacturing. However, highly-efficient removal of acetylene while avoiding overhydrogenation poses a huge challenge, especially in the front-end configurations containing excess H₂ and C₂H₄. To address the issue, our work aims to construct isolated active sites by modifying alumina-supported palladium (Pd/Al₂O₃) with Zeolite Socony Mobil-5 (ZSM-5) characterized by uniform micropores, which would spatially separate active metals without shielding them. A series of Pd/Al₂O₃@mZSM-5 composites were synthesized by adjusting the mass ratio of Pd/Al₂O₃ to ZSM-5 (corresponding to m in Pd/Al₂O₃@mZSM-5, where m = 1:1, 1:2, 1:3). The modification effect is confirmed by various characterizations. In situ diffusion reflectance infrared Fourier transform spectra (DRIFTS) of carbon monoxide indicates that surface Pd species in Pd/Al₂O₃@1:3ZSM-5 are efficiently segregated by the ZSM-5 framework, forming isolated Pd active sites with a partial negative charge. As expected, Pd/Al₂O₃@mZSM-5 composites exhibit much-improved selectivity toward ethylene compared with that of Pd/Al₂O₃. Moreover, the higher the amount of ZSM-5, the greater the selectivity. Notably, Pd/Al₂O₃@1:3ZSM-5 with an ultralow Pd loading of 211 ppm demonstrates exceptional selectivity and extraordinary hydrogenation activity within a broad operating temperature window of 125–250 °C. Specifically, it achieves near-complete conversion at 125 °C and delivers an outstanding specific activity of 8552 mol_C2H2 mol_Pd⁻¹ h⁻¹ at 100 °C, the highest value ever reported under comparable selectivity. Additionally, control experiments using amorphous silica (aSiO₂) and mesoporous Santa Barbara Amorphous-15 (SBA-15) as structural analogs of ZSM-5 highlight the irreplaceable role of microporous architecture in modifying Pd/Al₂O₃ to optimize the performance of acetylene semihydrogenation. According to in situ C₂H₄-DRIFTS, relative to Pd/Al₂O₃, the intensity of 2σ-bonded C₂H₄ is significantly suppressed on Pd/Al₂O₃@1:3ZSM-5 due to the isolated Pd active sites, which accounts for its excellent selectivity.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"696 ","pages":"Article 137907"},"PeriodicalIF":9.4,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144105069","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Hydrazide chemistry for durable, dendrite-free zinc anodes: Insights into solvation structures and electrolyte interfaces","authors":"Tianshi Wang ,&nbsp;Yu Guan ,&nbsp;Guolang Zhou ,&nbsp;Chong Zhao ,&nbsp;Cheng Liu ,&nbsp;Le Xu ,&nbsp;Zhipeng Cheng ,&nbsp;Shaoqian Jia ,&nbsp;Xiaozhe Li ,&nbsp;Zhichao Zhang ,&nbsp;Suyun Huang ,&nbsp;Qingxi Chen ,&nbsp;Xiyan Peng ,&nbsp;Yue Kong ,&nbsp;Fuqiang Shen ,&nbsp;Qiaofen Han ,&nbsp;Lili Zhang","doi":"10.1016/j.jcis.2025.137899","DOIUrl":"10.1016/j.jcis.2025.137899","url":null,"abstract":"<div><div>The practical application of aqueous Zn-ion batteries (AZIBs) is impeded by intrinsic limitations of Zn metal anode. Herein, benzoyl hydrazine (BH), incorporating multiple functional groups, serves as an electrolyte additive to mitigate interfacial side reactions and thereby enhancing its cycling durability. Experimental characterizations incorporating with theoretical simulations reveal that the BH molecule can not only reconstruct the solvation configuration by replacing the coordinated water of hydrated Zn²⁺, but strengthen hydrogen-bond network by forming strong hydrogen bonds, thus suppressing proton transport and active water decomposition. Additionally, BH molecules adsorb onto the Zn anode surface, establishing a versatile protective interfacial layer: hydrophobic benzene ring ligand can impede the direct desolvation of [Zn(H₂O)₆]²⁺ on the anode surface; nucleophilic sites coordinate desolvated Zn²⁺, modulating its flux to promote uniform Zn deposition and stripping. Consequently, Zn//Zn cells with low dosage of BH display a extended cycle life of 1200 h, and Zn//Cu cells run stably for 600 h with maintaining a high coulombic efficiency of 99.55 %. Moreover, Zn//MnO₂ full cells with 10 mM BH exhibited superior capacity retention after 1400 cycles. This work proposes a practical strategy by harnessing hydrazide chemistry to facilitate the development of AZIBs.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"697 ","pages":"Article 137899"},"PeriodicalIF":9.4,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088767","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"In situ regulating the accessibility and structure of Fe-based catalytic sites to break trade-off between the activity and stability for oxygen reduction","authors":"Jianglin Chen ,&nbsp;Jinyan Wu ,&nbsp;Chaozhong Guo ,&nbsp;Xiaoyu Dong ,&nbsp;Chenyang Shu ,&nbsp;Liumei Teng ,&nbsp;Yao Liu ,&nbsp;Hongdian Chen ,&nbsp;Rong Jin ,&nbsp;Caiyi Jiang ,&nbsp;Junjie Zhou ,&nbsp;Yujun Si ,&nbsp;Honglin Li ,&nbsp;Yong Pang","doi":"10.1016/j.jcis.2025.137910","DOIUrl":"10.1016/j.jcis.2025.137910","url":null,"abstract":"<div><div>How to synchronously boost the activity and stability of Fe/N-doped carbons (Fe-N-Ce-N-C) for oxygen reduction reaction (ORR) becomes important to promote their commercial applications. Here we synthesize a Fe-N-Ce-N-C catalyst by secondary sintering and removing endogenous CeO₂ nanoparticles to <em>in situ</em> regulate the accessibility and structure of N and O atoms coordinated Fe sites (FeN₂O₂). Theoretical studies indicate that the electron density distribution surrounding the Fe atom in FeN₂O₂ sites exhibits significant differences compared to that in FeN₄, inducing a downward shift of the Fe d-band center. FeN₂O₂ sites present a reduced free energy compared to FeN₄ sites, which contributes to an improved ORR catalytic activity. The Fe-N-Ce-N-C catalyst demonstrates a half-wave potential (<em>E</em>_1/2) of ∼0.906 V (<em>versus</em> RHE) and only 2.2 % reduction of <em>E</em>_1/2 (20 mV) after 30 k cycles of accelerated aging tests, revealing the superior ORR activity and stability in alkaline solution. The home-made zinc–air battery with the target catalyst delivers a high peak power density of 241.1 mW cm⁻² and a low voltage gap of 78.8 mV at 10 mA cm⁻². This work can provide an idea for obtaining available non-precious Fe-based electrocatalysts with a trade-off between activity and stability.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"697 ","pages":"Article 137910"},"PeriodicalIF":9.4,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144098827","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Sm3+ doped Na3V2-xSmx(PO4)3@C cathode for high-performance sodium ion batteries: Towards optimized sodium storage kinetics and cycling stability","authors":"Zhiqiang Lv ,&nbsp;Zijian You ,&nbsp;Xiang Zhang ,&nbsp;Yanbin Xu ,&nbsp;Yuming Cui ,&nbsp;Zhenglong Yang ,&nbsp;Bin Fang","doi":"10.1016/j.jcis.2025.137906","DOIUrl":"10.1016/j.jcis.2025.137906","url":null,"abstract":"<div><div>Na₃V₂(PO₄)₃ is considered a promising cathode material for high-performance sodium ion batteries due to its high operating voltage, fast ion diffusion and exceptionally stable crystal structure. However, its low intrinsic electronic conductivity remains a challenge for large-scale applications. In this study, a Sm³⁺-doped strategy is proposed to enhance its high-rate capacity and cycling stability. Theoretical calculations and charge transfer kinetics tests demonstrate that Sm³⁺ doping can reduce the band gap and Na⁺ diffusion energy barrier, thereby effectively enhancing electron conduction and Na⁺ migration. Moreover, the reduced integrated-crystal orbital Hamilton population (ICOHP) of Sm-O bond indicates improved structural stability of the crystal structure. Consequently, the synthesized Sm0.05-NVP@C exhibits outstanding rate capacities and cycling stabilities, delivering excellent reversible capacities of 103.26 and 72.81mAh g⁻¹ at 1C and 40C. Moreover, it demonstrates remarkable capacity retention of 92.56 % at 10C after 1250 cycles. Notably, in-situ XRD reveals a highly reversible bi-phase transition reaction mechanism between Na₃V_1.95Sm_0.05(PO₄)₃ and NaV_1.95Sm_0.05(PO₄)₃. This study highlights the great potential of Na₃V₂(PO₄)₃ cathode for achieving high-rate performance and long-term stability in sodium-ion batteries.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"696 ","pages":"Article 137906"},"PeriodicalIF":9.4,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144089740","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tuning oxygen molecule passivation and transfer on the catalyst surface for highly efficient hydrogen evolution from formaldehyde","authors":"Liangjun Cai ,&nbsp;Yang Wang ,&nbsp;Sili Ren ,&nbsp;Hongxia Liu ,&nbsp;Ding Zhang ,&nbsp;Xiaoxiao Yan","doi":"10.1016/j.jcis.2025.137905","DOIUrl":"10.1016/j.jcis.2025.137905","url":null,"abstract":"<div><div>In hydrogen evolution reactions (HER), hydrogen–oxygen recombination reaction typically reduces the hydrogen generation rate. However, in the HER from formaldehyde, un-dissociated oxygen molecules can promote hydrogen generation. In this paper, a series of PdZn/g-C₃N₄ alloy catalysts were synthesized, and by varying the catalyst composition successfully regulated the reactive sites and surface-interface behaviors, thus enhancing the HER rate. Under optimal conditions (1.5 M NaOH, 2.0 M HCHO, Pd₁Zn₁/g-C₃N₄), the Pd₁Zn₁ alloy catalyst exhibits the highest catalytic activity for hydrogen evolution reaction, with a hydrogen evolution rate of 422.86 μmol·h⁻¹. Mechanistic study of hydrogen production from formaldehyde revealed that O₂ molecules are converted into reactive oxygen species HOO⁻, which then react with formaldehyde to produce hydrogen. The adsorption energies of formaldehyde and oxygen molecules, as well as the O₂ dissociation energy barrier, vary significantly with the PdZn alloy compositions, affecting O₂ chemical behavior, impeding O₂ dissociation, and accelerating the transfer of active species. The results of theoretical calculations indicate that on the surface of the Pd₁Zn₁/g-C₃N₄ alloy catalyst, oxygen molecules possess an appropriate adsorption energy and a relatively high dissociation energy barrier. This is conducive to the formation of oxygen-containing active species. Meanwhile, the coordination between metal atoms promotes the efficient transfer of photogenerated electrons and prolongs the photoelectron lifetime. Thus, adjusting the PdZn alloy composition can effectively regulate and enhance the catalyst’s hydrogen production activity.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"697 ","pages":"Article 137905"},"PeriodicalIF":9.4,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144108192","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}