{"title":"Tailored acidity of silylated Pt/USY catalysts to regulate catalytic performances for phenol hydrogenation","authors":"Zhi Wang, Jun Chen, Gaolei Shi, Liuwei Shen, Xueqin Ma, Xingguang Zhang","doi":"10.1016/j.apcata.2026.120787","DOIUrl":"10.1016/j.apcata.2026.120787","url":null,"abstract":"<div><div>Pt-based catalysts supported on acidic zeolites are intensively utilized for selective hydrogenation reactions; yet the interplay between zeolite acidity and metal sites remains important research topics, because zeolites feature adjustable acidity (Brønsted/Lewis), strong (hydrothermal-)stability, and highly-ordered porosity for nanoconfinement and shape selectivity. This study systematically identifies the contribution of Brønsted (B) acids and Lewis (L) acid sites in Pt/USY catalysts tailored by controlled introduction of diethoxydimethylsilane (DEDMS, 0–5.0 % wt) for phenol hydrogenation to cyclohexanol and cyclohexanone. The modification declined B acid sites (from 145.8 over 1 %Pt/USY-1–14.7 μmol/g over 1 %Pt/5.0 %DEDMS-USY) and L acid sites (from 129.3 to 38.4 μmol/g). The reduction in B acid sites considerably suppressed phenol adsorption and thus decreased its conversion from 100 % (1 %Pt/USY-1) to 19.0 % (1 %Pt/5.0 %DEDMS-USY-1), and the reduction in L acid sites primarily suppressed the cyclohexanone adsorption and thus increased its selectivity from being undetectable (1 %Pt/USY-1) to 57.7 % (1 %Pt/5.0 %DEDMS-USY). The silylation could effectively tailor the catalytic activity and selectivity of Pt/USY catalysts and provides valuable insights for designing bifunctional catalysts in selective hydrogenation.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"712 ","pages":"Article 120787"},"PeriodicalIF":4.8,"publicationDate":"2026-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974650","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Changshun Deng , Chaoxiang Li , Haoyu Lu , Bingqing Ge , Weiping Ding
{"title":"Reaction pathways of MoVTeNbO directed by Te defects for selective oxidation of toluene","authors":"Changshun Deng , Chaoxiang Li , Haoyu Lu , Bingqing Ge , Weiping Ding","doi":"10.1016/j.apcata.2026.120783","DOIUrl":"10.1016/j.apcata.2026.120783","url":null,"abstract":"<div><div>MoVTeNbO is a famous oxide of multi-component and effective for gaseous toluene oxidation to benzaldehyde, but exhibits catalytic properties highly sensitive to composition and surface properties. Here, we report the regulation of catalytic properties of MoVTeNbO by Te defects tuned in hydrothermal synthesis, even in the same bulk crystal structure of M1 phase, leading to significant difference in catalytic performance for selective oxidation of toluene using air as oxidant. The catalyst MoVTeNbO-1 in nano brick shape exhibits weaker redox capacity and acidity as well as lower contents of surface V<sup>5 +</sup> and electrophilic oxygen species, giving rise to a conversion of toluene exceeding 8 % with a selectivity of 73 % to benzaldehyde at 350 °C. Nevertheless, the stronger oxidation capacity of MoVTeNbO-2 in nano firewood shape shows an outstanding activity for toluene oxidation at a conversion of ∼84 % and a selectivity more than 60 % to maleic anhydride at the same temperature. Further study indicates that much more Te defects in MoVTeNbO-2 play a key role for the regulation of its surface properties and direct the catalyst for toluene oxidation following totally different pathways of conversion. Results of characterizations including kinetics <em>in-situ</em> spectroscopy also indicate that the toluene oxidation over nano brick MoVTeNbO-1 follows an Eley-Rideal mechanism, but the toluene oxidation over nano firewood shaped MoVTeNbO-2 complies with a Langmuir-Hinshelwood mechanism.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"712 ","pages":"Article 120783"},"PeriodicalIF":4.8,"publicationDate":"2026-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974700","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Elsayed G. Blall , Rafah Mohammed Thyab , Ahmed H. Abdel-Salam , Ahmed Morsy , Leonara de Oliveira Moura , Asmaa Mohamed , Ashraf Morsy
{"title":"Chalcone-based catalysts and functional nanomaterials for heavy-metal remediation: Mechanistic insights and environmental applications","authors":"Elsayed G. Blall , Rafah Mohammed Thyab , Ahmed H. Abdel-Salam , Ahmed Morsy , Leonara de Oliveira Moura , Asmaa Mohamed , Ashraf Morsy","doi":"10.1016/j.apcata.2026.120774","DOIUrl":"10.1016/j.apcata.2026.120774","url":null,"abstract":"<div><div>Heavy-metal contamination remains one of the most persistent global environmental challenges due to its toxicity, non-biodegradability, and accumulation in ecosystems. Conventional remediation techniques often struggle to achieve sustainable, selective, and efficient removal under realistic conditions. Chalcones, a subclass of flavonoids characterized by an α,β-unsaturated carbonyl framework, have recently attracted attention as multifunctional ligands capable of chelation, redox mediation, and surface interactions with transition metals. Recent studies have elucidated the mechanistic role of chalcone-based accelerators in cementation processes, particularly in enhancing catalytic activity and electron-transfer pathways for metal recovery. In parallel, chalcone-functionalized nanoparticles and hybrid nanocomposites have been reported to integrate adsorption, complexation, and redox mechanisms, enabling efficient removal of heavy metals such as Pb(II), Cd(II), and Cr(VI). Comparative analyses of adsorption kinetics, thermodynamic behavior, and regeneration performance reveal distinct advantages of chalcone-derived systems over conventional adsorbents, supported by molecular-level insights from density functional theory (DFT) and spectroscopic investigations. Current research trends indicate growing potential for incorporating chalcone-based nanomaterials into scalable water-treatment and resource-recovery applications, particularly through green synthesis approaches, stability enhancement, and cost-effective implementation.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"712 ","pages":"Article 120774"},"PeriodicalIF":4.8,"publicationDate":"2026-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145903923","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Young Woo Kim , Eun-Jeong Kim , Sungjoon Kweon , Ho Jin Lee , Min Bum Park , Eun Duck Park , Chae-Ho Shin , Yongju Yun
{"title":"Tailoring support defects in Ru/yttria–ceria catalysts for efficient and durable ammonia decomposition","authors":"Young Woo Kim , Eun-Jeong Kim , Sungjoon Kweon , Ho Jin Lee , Min Bum Park , Eun Duck Park , Chae-Ho Shin , Yongju Yun","doi":"10.1016/j.apcata.2026.120791","DOIUrl":"10.1016/j.apcata.2026.120791","url":null,"abstract":"<div><div>The catalytic decomposition of ammonia (NH<sub>3</sub>) offers a carbon-free route for on-demand hydrogen production; however, achieving high activity and durability under moderate temperatures remains challenging. Ru-based catalysts supported on CeO<sub>2</sub> exhibit excellent intrinsic activity, but their performance is limited by insufficient defect density and moderate metal–support interaction. Here, we establish a structure–defect–interaction–performance relationship for Ru catalysts supported on yttria–ceria mixed oxides (Ru/<em>a</em>Y-CeO<sub>x</sub>) by systematically varying the Y content of the support. Incorporating Y<sup>3+</sup> into the CeO<sub>2</sub> lattice induces lattice distortion and oxygen vacancies while preserving the fluorite structure up to moderate Y contents. These structural defects strengthen the Ru–O–Ce interfacial bonding, facilitate electron transfer, and enhance the surface basicity of the support. The Ru/50Y-CeO<sub>x</sub> catalyst achieves 80 % NH<sub>3</sub> conversion at 450 °C with a hydrogen formation rate of 10.8 mmol∙g<sub>cat</sub><sup>−1</sup>∙min<sup>−1</sup> and maintains stable operation for 168 h without deactivation. This superior performance is attributed to the optimal defect density that maximizes Ru–support coupling, accelerates recombinative N<sub>2</sub> desorption, and mitigates H<sub>2</sub> poisoning. These findings highlight that tailoring lattice defects in rare-earth oxide supports provides a rational strategy for designing efficient and durable Ru-based catalysts for carbon-free hydrogen production.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"712 ","pages":"Article 120791"},"PeriodicalIF":4.8,"publicationDate":"2026-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974116","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ZeYi Ren , Hui Bai , Lingyun Fang , XiaoMei Ma , Beibei Sun , Yujie Zhang , Fengqin Tang , JunYi Chen
{"title":"Cerium-doped medium-entropy layered double hydroxides with abundant oxygen vacancies for efficient peroxymonosulfate activation in water purification","authors":"ZeYi Ren , Hui Bai , Lingyun Fang , XiaoMei Ma , Beibei Sun , Yujie Zhang , Fengqin Tang , JunYi Chen","doi":"10.1016/j.apcata.2026.120790","DOIUrl":"10.1016/j.apcata.2026.120790","url":null,"abstract":"<div><div>The rational design of efficient heterogeneous catalysts for peroxymonosulfate (PMS) activation is of great significance for advanced oxidation processes in environmental remediation. Herein, daisy-like quaternary medium-entropy layered double hydroxides (Ce<sub>0.4</sub>-MeLDHs) were synthesized via strategic cerium incorporation into the NiCoFe-LDH framework. Ce doping effectively enriched oxygen vacancies and modulated the electronic structure, thereby boosting PMS uptake and activation. Under optimal conditions (pH = 7, PMS =100 mg/L, catalyst = 100 mg/L), Ce<sub>0.4</sub>-MeLDHs achieved 96.6 % removal of methylene blue (MB, 20 mg/L) within 12 min, with a reaction rate constant 1.4-fold higher than pristine NiCoFe-LDH. Radical scavenging and electron paramagnetic resonance analyses revealed that <sup>1</sup>O<sub>2</sub> dominated MB degradation, with •OH and •O<sup>–</sup><sub>2</sub> providing synergistic contributions. The superior catalytic activity was ascribed to the interplay between Ce<sup>3+</sup>/Ce<sup>4+</sup> redox cycling, transition-metal redox couples (Ni<sup>2+</sup>/Ni<sup>3+</sup>, Co<sup>2+</sup>/Co<sup>3+</sup>, Fe<sup>2+</sup>/Fe<sup>3+</sup>), and abundant oxygen vacancies (OVs). Furthermore, Ce<sub>0.4</sub>-MeLDHs exhibited excellent stability, maintaining > 90 % efficiency after four cycles, and broad-spectrum activity in real water matrices. This work highlights rare-earth doping as an effective strategy to construct entropy-stabilized, oxygen-vacancy-rich LDHs with great promise for sustainable water purification.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"712 ","pages":"Article 120790"},"PeriodicalIF":4.8,"publicationDate":"2026-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974114","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Exploring the catalytic chan-lam coupling reaction of N-Arylation of amines using heterogeneous thiophene schiff base-Ni-bipy complex on mesoporous MCM-41","authors":"Narmatha Venkatesan, Rajashri Varadarasu, Jayapratha Gunasekaran, Shanmuga Bharathi Kuppannan","doi":"10.1016/j.apcata.2026.120793","DOIUrl":"10.1016/j.apcata.2026.120793","url":null,"abstract":"<div><div>The present work is planned to examine the <em>N</em>-arylation of amines using well-defined heterogeneous catalyst. For this process, the mixed thiophene Schiff base and 2,2’-bipyridyl based nickel (II) complex was embedded on hexagonally aligned mesoporous MCM-41 and it has been characterized by the Fourier transform infra-red spectroscopy (FT-IR), powder X-ray diffraction (PXRD), ultraviolet-visible diffuse reflectance spectroscopy (UV-Vis DRS), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), elemental mapping, inductively coupled plasma-optical emission spectrometry (ICP-OES), transmission electron microscope (TEM), thermogravimetric analysis (TGA), N<sub>2</sub> adsorption–desorption isotherm (BET), and X-ray photoelectron spectroscopy (XPS) techniques. The catalytic efficiency of the compound was assessed in <em>N</em>-arylation of amines using phenylboronic acid with various substituted amines (viz. electron donating/ withdrawing, fused ring, heterocyclic and aliphatic substituents), K<sub>2</sub>CO<sub>3</sub> under reflux using toluene solvent for 2 h which resulted in excellent yield up to 95 % with independent of their substituents nature. Moreover, hot filtration and recyclability tests of our catalyst validated the heterogeneity nature which worked upto five sequential cycles with maximum stability in the catalytic reaction. A plausible reaction mechanism for the <em>N</em>-arylation of amines and the comparison of catalytic efficiency of our catalyst against some notable reported catalysts were also discussed.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"712 ","pages":"Article 120793"},"PeriodicalIF":4.8,"publicationDate":"2026-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146035280","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hongshang Wang , Jingkai Ma , Ruihan Lv , Ji Mi , Wenjun Fang
{"title":"Efficient hydrogen generation via steam reforming of ultra-stable emulsified hydrocarbon fuel catalyzed by NixPt1-x/Al2O3","authors":"Hongshang Wang , Jingkai Ma , Ruihan Lv , Ji Mi , Wenjun Fang","doi":"10.1016/j.apcata.2026.120794","DOIUrl":"10.1016/j.apcata.2026.120794","url":null,"abstract":"<div><div>Traditional steam reforming technology encounters two primary challenges: catalyst deactivation and fuel system instability, which limit its hydrogen production efficiency and potential applications. This work addresses these challenges through the concurrent development of novel catalysts and highly stable fuel emulsions. In this work, ultra-stable quasi-homogeneous “water + JP-10/RP-3” systems were formulated utilizing binary Span 80/Tween 80 emulsifiers. The alloy-structured Ni<sub>0.93</sub>Pt<sub>0.07</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst was synthesized via stirred impregnation followed by annealing. The catalyst demonstrated superior reforming efficiency and resistance to coking: with exo-tetrahydrodicyclopentadiene (JP-10,one of jet fuels) at 740 °C, a gas yield of 28.8 wt% and a hydrogen output of 4.68 mmol·g<sup>−1</sup> were achieved alongside a consistent 20 % level of aromatic coke precursors. Furthermore, its capability with complex fuels was affirmed by reforming RP-3 aviation kerosene at 700 °C, which yielded 3.48 mmol·g<sup>−1</sup> of H<sub>2</sub>. By combining steam reforming performance tests with density functional theory (DFT) calculations, and X-ray absorption fine structure (XAFS) analysis, this study clarifies the dual synergistic effects that contribute to its exceptional performance: (1) Platinum-induced electron-rich nickel significantly decreases the adsorption energy of critical intermediates, hence improving the efficiency of C-H bond activation. (2) The Pt addition markedly diminishes carbon deposition by reducing the tendency of CH<sub><em>x</em></sub>* intermediates to undergo further dehydrogenation into carbonaceous deposits, facilitating their effective removal.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"712 ","pages":"Article 120794"},"PeriodicalIF":4.8,"publicationDate":"2026-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146035602","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Ligand-engineered cobalt precursors toward enhanced catalytic activity of Co@S-1 zeolite in toluene oxidation","authors":"Shengnan Xu, Yu Yu, Fuxin Wang, Jiande Hu, Zixiang Li, Guojun Lv","doi":"10.1016/j.apcata.2026.120784","DOIUrl":"10.1016/j.apcata.2026.120784","url":null,"abstract":"<div><div>Cobalt-doped zeolite catalysts have been identified as a potentially viable non-precious metal alternative for toluene oxidation, exhibiting characteristics reminiscent of noble metals, such as the ability to activate C-H bonds, abundance, and minimal adverse environmental impact. However, the catalytic activity is greatly reliant on the diversity of cobalt species embedded within the zeolite framework. To address this, a ligand-engineering strategy was utilized to precisely control the coordination environment of the cobalt precursor, thereby regulating the resulting cobalt species and accordingly the catalytic activity of cobalt-doped zeolite catalysts. Four distinct Co@S-1 zeolites were synthesized with disparate ligands including ethylenediamine, water, ammonia water and acetylacetone, and meanwhile applied as heterogeneous catalysts for the selective oxidation of toluene with molecular oxygen as oxidant. Among them, the Co@S-1(EDA) zeolite catalyst synthesized with ethylenediamine demonstrated superior catalytic reaction performance, achieving a toluene conversion of 63.8 % with a benzaldehyde selectivity of 68.5 % within 6 h of reaction. This eminent catalytic oxidation ability for Co@S-1(EDA) zeolite catalyst is mainly ascribed to its largest Co<sup>2+</sup>/Co<sup>3+</sup> ratio, its most oxygen vacancy amount and its largest external surface area. Furthermore, the Co@S-1(EDA) zeolite catalyst exhibited excellent re-usability, maintaining its activity over five consecutive catalytic cycles. This study emphasizes ligand engineering as an effective approach to create highly efficient and stable cobalt-based zeolite catalysts for selective hydrocarbon oxidation reactions.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"712 ","pages":"Article 120784"},"PeriodicalIF":4.8,"publicationDate":"2026-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974697","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Synergy of confinement effect and oxygen vacancy in carboxymethyl-β-cyclodextrin-intercalated CoAl-LDH for boosting selective aerobic oxidation of alcohols in water","authors":"Fang Fang, Dongping Sun, Xinhua Peng","doi":"10.1016/j.apcata.2026.120771","DOIUrl":"10.1016/j.apcata.2026.120771","url":null,"abstract":"<div><div>Selective catalytic aerobic oxidation of alcohols into aldehydes and ketones using water as solvent and layered double hydroxides as alkaline catalyst exemplifies both atom economy and environmental benignity. In this work, we initially synthesized oxygen vacancy-rich monolayer m-CoAl-LDH nanosheets through a facile direct synthesis method. Then, by reassembling the CMCD anions with m-CoAl-LDH layers to form an oxygen vacancy-rich heterogeneous CMCD-CoAl-LDH intercalation hybrid. We investigated the application of CMCD-CoAl-LDH in the aerobic oxidation of alcohol in water, and examined the structure-activity relationship. The oxygen vacancy defect sites on the LDH layers activate both oxygen and alcohol molecules. Concurrently, CMCD with LDH layers collaboratively form a confined environment, exerting the confinement effect to achieve highly efficient and selective aerobic oxidation. The adsorption and surface reaction of benzyl alcohol on the catalyst in an O<sub>2</sub> atmosphere were investigated by in situ DRIFT spectroscopy. DFT calculation of adsorption energy reveals that oxygen vacancies serve as the primary sites for the adsorption of benzyl alcohol and oxygen molecules. This catalyst system demonstrates excellent compatibility with green aqueous media and significantly promotes the aerobic oxidation of alcohol. It provides a feasible paradigm of integrating supramolecular chemistry with materials chemistry to address challenges in catalysis.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"712 ","pages":"Article 120771"},"PeriodicalIF":4.8,"publicationDate":"2026-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941062","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Thomas Häber , Sui Wan , Samuel Struzek , Camilo Cárdenas , Anna Zimina , Florian Maurer , Patrick Lott , Rainer Suntz , Jan-Dierk Grunwaldt , Olaf Deutschmann
{"title":"Novel advanced channel reactor for spatio-temporal activity and catalyst state correlations applied for the reduction of NO by CO over Pt/Al2O3","authors":"Thomas Häber , Sui Wan , Samuel Struzek , Camilo Cárdenas , Anna Zimina , Florian Maurer , Patrick Lott , Rainer Suntz , Jan-Dierk Grunwaldt , Olaf Deutschmann","doi":"10.1016/j.apcata.2025.120748","DOIUrl":"10.1016/j.apcata.2025.120748","url":null,"abstract":"<div><div>The correlation of space- and time-resolved measurements of catalytic activity with catalyst state is an invaluable tool to advance the understanding and development of complex catalytic systems under conditions relevant to technical applications. Such an approach is employed here to investigate the catalytic deactivation in the reduction of NO by CO over Pt/Al<sub>2</sub>O<sub>3</sub> on freshly reduced catalysts in a channel reactor and at concentrations typical for emission control. Planar laser-induced fluorescence (PLIF) is used to visualize the 2D concentration profiles and to derive space- and time-resolved NO conversion rates for different CO/NO ratios, temperatures and mass flow rates. The changes in catalytic activity are correlated with temporal and spatial changes in oxidation state determined by <em>operando</em> X-ray absorption spectroscopy (XAS) under the same conditions. The time scales of the changes in catalytic activity depend not only on the stoichiometry and temperature, but also on the position along the catalyst channel and differ significantly from the temporal changes of the oxidation state. The different time scales are discussed in the context of the known CO poisoning as well as the formation and storage of isocyanate on the support. Isocyanate formation temporarily counteracting CO poisoning could explain the differences in the observed time scales under different reaction conditions and at different locations on the catalyst.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"712 ","pages":"Article 120748"},"PeriodicalIF":4.8,"publicationDate":"2026-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145940922","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}