Yangzhi Xu , Zirui Gao , Yao Xu , Xuetao Qin , Xin Tang , Zhiwei Xie , Jinrong Zhang , Chuqiao Song , Siyu Yao , Wu Zhou , Ding Ma , Lili Lin
{"title":"Cu-supported nano-ZrZnOx as a highly active inverse catalyst for low temperature methanol synthesis from CO2 hydrogenation","authors":"Yangzhi Xu , Zirui Gao , Yao Xu , Xuetao Qin , Xin Tang , Zhiwei Xie , Jinrong Zhang , Chuqiao Song , Siyu Yao , Wu Zhou , Ding Ma , Lili Lin","doi":"10.1016/j.apcatb.2023.123656","DOIUrl":"10.1016/j.apcatb.2023.123656","url":null,"abstract":"<div><p>Hydrogenation of CO<sub>2</sub> into methanol at low-temperature on Cu-based catalysts is of great significance, but remains challenging to enhance activity. In this paper, we report an inverse catalyst constructed with nano-ZrZnO<sub>x</sub><span> supported on Cu particles with outstanding methanol synthesis performance at 220 ℃, two times higher than that of commercial Cu/ZnO/Al</span><sub>2</sub>O<sub>3</sub> catalysts under the same conditions. Detailed structure characterization and performance evaluation demonstrate that the ZrZnO<sub>x</sub> mixed oxide serves as the most active oxide-metal interface site for CO<sub>2</sub> hydrogenation. The ZrZnO<sub>x</sub>/Cu inverse catalyst increases the weak and medium CO<sub>2</sub> adsorption sites which are further demonstrated responsible to the methanol productivity. <em>In situ</em> DRIFTs studies reveal that the inverse interface accelerates the reduction of asymmetric formate intermediates and prevents the generation of CO. The combination of enhanced CO<sub>2</sub> activation capability and accelerated hydrogenation rate of intermediates over the ZrZnO<sub>x</sub>/Cu inverse catalyst probably contribute to the remarkable methanol synthesis performance from CO<sub>2</sub>.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"344 ","pages":"Article 123656"},"PeriodicalIF":22.1,"publicationDate":"2023-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139030625","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}
Wenjie He , Jing Xiong , Zhiling Tang , Yingli Wang , Xiong Wang , Hui Xu , Zhen Zhao , Jian Liu , Yuechang Wei
{"title":"Localized surface plasmon resonance effect of bismuth nanoparticles in Bi/TiO2 catalysts for boosting visible light-driven CO2 reduction to CH4","authors":"Wenjie He , Jing Xiong , Zhiling Tang , Yingli Wang , Xiong Wang , Hui Xu , Zhen Zhao , Jian Liu , Yuechang Wei","doi":"10.1016/j.apcatb.2023.123651","DOIUrl":"10.1016/j.apcatb.2023.123651","url":null,"abstract":"<div><p>Herein, the photocatalysts of metallic Bi-modified TiO<sub>2</sub><span> microsphere (namely BTO) were synthesized by one-pot solvothermal method. The localized surface plasmon resonance (LSPR) effect of introduced metallic Bi nanoparticles is beneficial to improve the absorption efficiency for visible light, and its surface hot electrons can donate to the valence band of TiO</span><sub>2</sub> for boosting the separation efficiency of light generated electron-hole pairs. BTO catalysts exhibit the super catalytic activity for visible light-driven CO<sub>2</sub> reduction with H<sub>2</sub>O to CH<sub>4</sub>. The formation amount and selectivity of CH<sub>4</sub> product over BTO-2 catalyst are 49.12 μmol g<sup>−1</sup> and 85.48 % for 4 h, respectively. Based on the results of in-situ DRIFTS and density functional theory calculation, the mechanism for photocatalytic CO<sub>2</sub> reduction is proposed: the visible light-driven LSPR effect on BTO catalyst can boost the key step of CO<sub>2</sub>* -to-HCO* for promoting selective generation of CH<sub>4</sub> product. It inspires the design of efficient photocatalysts for CO<sub>2</sub> conversion.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"344 ","pages":"Article 123651"},"PeriodicalIF":22.1,"publicationDate":"2023-12-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139030775","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}
Yuhan Long , Zhenhua Cao , Weiran Wu , Wenhao Liu , Peizhen Yang , Xuesong Zhan , Rongzhi Chen , Dongfang Liu , Wenli Huang
{"title":"Rational modulation of Fe single-atom electronic structure in a Fe-N2B4 configuration for preferential 1O2 generation in Fenton-like reactions","authors":"Yuhan Long , Zhenhua Cao , Weiran Wu , Wenhao Liu , Peizhen Yang , Xuesong Zhan , Rongzhi Chen , Dongfang Liu , Wenli Huang","doi":"10.1016/j.apcatb.2023.123643","DOIUrl":"10.1016/j.apcatb.2023.123643","url":null,"abstract":"<div><p>The important role of optimizing the coordination environment of single-atom catalysts (SACs) for selective production of singlet oxygen (<sup>1</sup>O<sub>2</sub>) in Fenton-like reactions is revealed. Herein, we introduce electron-depletion boron atoms to manipulate the coordination number and atom types of Fe site simultaneously and construct a six-coordination Fe-N<sub>2</sub>B<sub>4</sub> catalyst for peroxymonosulfte (PMS) activation. Particularly, it achieves 98.68% <sup>1</sup>O<sub>2</sub> generation selectivity superior to unregulated Fe-N<sub>4</sub><span> catalyst (64.57%), exhibiting an exceptional bisphenol A (BPA) degradation performance with a reaction rate constant of 0.249 min</span><sup>−1</sup>. Experimental and theoretical results unveil that the tailored electronic structure of Fe not only enhances the adsorption selectivity of terminal oxygen atoms in PMS and alters the reaction pathway preference, but also facilitates the electron donation from PMS and lowers the energy barrier for <sup>1</sup>O<sub>2</sub> generation. This work provides a universal strategy for rational and precise modulation of SACs for specific reactive species conversion in environment remediation.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"344 ","pages":"Article 123643"},"PeriodicalIF":22.1,"publicationDate":"2023-12-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138991171","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}
Bangrong Ming , Tongtong Jia , Yufan Zhang , Jikun Li , Chuncheng Chen , Wenjing Song , Jincai Zhao
{"title":"Steering single-site metallaphotocatalytic pathway by accumulated electron on carbon nitride support","authors":"Bangrong Ming , Tongtong Jia , Yufan Zhang , Jikun Li , Chuncheng Chen , Wenjing Song , Jincai Zhao","doi":"10.1016/j.apcatb.2023.123653","DOIUrl":"10.1016/j.apcatb.2023.123653","url":null,"abstract":"<div><p><span>Organic halide transformation is of high importance for fine chemical synthesis and environmental remediation. Integrated photocatalytic platforms open up distinctive reaction pathway for carbon-halogen bond activation/reconstruction. Herein we reveal carbon nitride (CN)-ligated single atom nickel (Ni</span><sub>1</sub>/CN), with accumulated electron on the CN, paves Ni-mediated electron-proton transfer, enabling hydrodehalogenation, along with the catalytic carbon–oxygen (C–O) coupling. The preference for hydrodehalogenation positively correlates with density of electron on CN. EPR measurements suggest photo-generated Ni<sup>I</sup><span><span> interacts with aryl halides, followed by electron transfer or reductive elimination<span> to give different products. Further kinetic studies on hydrodehalogenation/C–O coupling show the reaction orders of 0.1/0.5 in aryl halide and 1.5/0.03 in (CN) electron, unveiling rate-determining step as </span></span>oxidative addition to Ni</span><sup>I</sup> and (CN) electron transfer for the two conversions. Our work advances in modulating aryl halide conversion by carrier accumulation on the photoactive support and guides metallaphotocatalytic platform design/operation toward target transformations.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"344 ","pages":"Article 123653"},"PeriodicalIF":22.1,"publicationDate":"2023-12-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139020309","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":"Steering Single-Site Metallaphotocatalytic Pathway by Accumulated Electron on Carbon Nitride Support","authors":"Bangrong Ming, Tongtong Jia, Yufan Zhang, Jikun Li, Chuncheng Chen, Wenjing Song, Jincai Zhao","doi":"10.1016/j.apcatb.2023.123653","DOIUrl":"https://doi.org/10.1016/j.apcatb.2023.123653","url":null,"abstract":"<p>Organic halide transformation is of high importance for fine chemical synthesis and environmental remediation. Integrated photocatalytic platforms open up distinctive reaction pathway for carbon-halogen bond activation/reconstruction. Herein we reveal carbon nitride (CN)-ligated single atom nickel (Ni<sub>1</sub>/CN), with accumulated electron on the CN, paves Ni-mediated electron-proton transfer, enabling hydrodehalogenation, along with the catalytic carbon–oxygen (C–O) coupling. The preference for hydrodehalogenation positively correlates with density of electron on CN. EPR measurements suggest photo-generated Ni<sup>I</sup> interacts with aryl halides, followed by electron transfer or reductive elimination to give different products. Further kinetic studies on hydrodehalogenation/ C–O coupling show the reaction orders of 0.1/0.5 in aryl halide and 1.5/0.03 in (CN) electron, unveiling rate-determining step as oxidative addition to Ni<sup>I</sup> and (CN) electron transfer for the two conversions. Our work advances in modulating aryl halide conversion by carrier accumulation on the photoactive support and guides metallaphotocatalytic platform design/operation toward target transformations.</p>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"61 1","pages":""},"PeriodicalIF":22.1,"publicationDate":"2023-12-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139030659","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}
Pianpian Zhang , Tingting Sun , Rong Jiang , Tianyu Zheng , Qingmei Xu , Ruanbo Hu , Xinxin Wang , Kang Wang , Lianbin Xu , Dingsheng Wang , Jianzhuang Jiang
{"title":"A robust asymmetric diatomic electrocatalyst for oxygen reduction reaction in both acidic and alkaline media","authors":"Pianpian Zhang , Tingting Sun , Rong Jiang , Tianyu Zheng , Qingmei Xu , Ruanbo Hu , Xinxin Wang , Kang Wang , Lianbin Xu , Dingsheng Wang , Jianzhuang Jiang","doi":"10.1016/j.apcatb.2023.123645","DOIUrl":"10.1016/j.apcatb.2023.123645","url":null,"abstract":"<div><p><span>Herein, an asymmetric diatomic site oxygen reduction reaction (ORR) electrocatalyst with atomically dispersed Fe and Cu species co-anchored on porous nitrogen-doped polyhedra carbon was successfully prepared through a facile cooperation of post-adsorption and two-step pyrolysis method. Density functional theory (DFT) calculations reveal that the asymmetric FeCu dual atomic site experiences a symmetry destruction of electron transfer due to the existing Cu-N</span><sub>4</sub> sites and thus results in the electron redistribution in Fe<sub>SA</sub>Cu<sub>SA</sub>/NC, contributing significantly to the optimization of intermediates adsorption and acceleration of kinetics during ORR process. Attributed to the structural advantages of Fe<sub>SA</sub>-N<sub>4</sub>&Cu<sub>SA</sub>-N<sub>4</sub> sites and highly porous carbon matrix, the Fe<sub>SA</sub>Cu<sub>SA</sub>/NC catalyst exhibits excellent electrocatalytic ORR performance with half-wave potentials (<em>E</em><sub><em>1/2</em></sub>) of 0.86 and 0.88 V versus reversible hydrogen electrode in 0.1 M HClO<sub>4</sub> and 0.1 M KOH solutions as well as high durability. Moreover, Fe<sub>SA</sub>Cu<sub>SA</sub>/NC-based H<sub>2</sub>/O<sub>2</sub> fuel cell and zinc-air battery present superior performance with high peak power density.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"344 ","pages":"Article 123645"},"PeriodicalIF":22.1,"publicationDate":"2023-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138821334","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}
Yuxuan Ma , Dan He , Quansheng Liu , Shukun Le , Xiaojing Wang
{"title":"A S-type 2D/2D heterojunction via intercalating ultrathin g-C3N4 into NH4V4O10 nanosheets and the boosted removal of ciprofloxacin","authors":"Yuxuan Ma , Dan He , Quansheng Liu , Shukun Le , Xiaojing Wang","doi":"10.1016/j.apcatb.2023.123642","DOIUrl":"10.1016/j.apcatb.2023.123642","url":null,"abstract":"<div><p>Exploring cheap, eco-friendliness, and highly efficiency photocatalysts for improving the degradation performance of ciprofloxacin (CIP) is a challenge in the environmental remediation field. Herein, 2D/2D ultrathin g-C<sub>3</sub>N<sub>4</sub>/NH<sub>4</sub>V<sub>4</sub>O<sub>10</sub> (CNNS/NH<sub>4</sub>V<sub>4</sub>O<sub>10</sub>) heterojunction is successfully prepared by intercalating g-C<sub>3</sub>N<sub>4</sub> nanosheets into the ultrathin NH<sub>4</sub>V<sub>4</sub>O<sub>10</sub><span> nanobelts. For the optimized 50-CNNS/NH</span><sub>4</sub>V<sub>4</sub>O<sub>10</sub>, the removal rate is 92% for 10 mg·L<sup>−1</sup><span> CIP under simulated solar light, far better than the separated components CNNS and NH</span><sub>4</sub>V<sub>4</sub>O<sub>10</sub>. Moreover, the wide degraded concentration of CIP ranges from 5 to 40 mg·L<sup>−1</sup> devotes a prospect of practical application. The mechanism investigation confirms the intercalating action can break the interlaminar bonding linkage of NH<sub>4</sub>, which increases the surface NH<sub>4</sub><sup>+</sup> content and promotes the steered adsorption capacity toward ciprofloxacin through binding to F<sup>-</sup><span> in CIP via H-bonding. This work provides a novel design idea for constructing 2D/2D intercalated nanocomposite<span> for the application in the removal of the deleterious fluoric-containing organic pollutants in water environment.</span></span></p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"344 ","pages":"Article 123642"},"PeriodicalIF":22.1,"publicationDate":"2023-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139017277","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}
Meijun Li , Junyan Zhang , Stephen C. Purdy , Fan Lin , Kinga A. Unocic , Michael Cordon , Zili Wu , Huamin Wang , Jacklyn Hall , A. Jeremy Kropf , Theodore R. Krause , Brian Davison , Zhenglong Li , Andrew D. Sutton
{"title":"Tailoring olefin distribution via tuning rare earth metals in bifunctional Cu-RE/beta-zeolite catalysts for ethanol upgrading","authors":"Meijun Li , Junyan Zhang , Stephen C. Purdy , Fan Lin , Kinga A. Unocic , Michael Cordon , Zili Wu , Huamin Wang , Jacklyn Hall , A. Jeremy Kropf , Theodore R. Krause , Brian Davison , Zhenglong Li , Andrew D. Sutton","doi":"10.1016/j.apcatb.2023.123648","DOIUrl":"10.1016/j.apcatb.2023.123648","url":null,"abstract":"<div><p>Bioethanol to middle distillate technologies have offered a unique solution to produce renewable aviation fuel for decarbonizing the hard-to-electrify sectors. Here, we have developed the series of bimetallic Cu- and rare earth-containing (RE) Beta zeolite catalysts that yield high C<sub>3+</sub><span> alkene<span> selectivity from ethanol upgrading (>80% selectivity at ∼100% conversion, 623 K). The formation rates of butene isomers to C</span></span><sub>5+</sub> alkenes are linearly correlated with the strength of Lewis acidic RE identity, which follows the sequence of Yb<sub>12</sub>/Beta >Y<sub>7</sub>/Beta > Gd<sub>12</sub>/Beta > Ce<sub>10</sub>/Beta > La<sub>12</sub>/Beta. Rate measurements indicate that the RE selection plays the vital role in altering the rate of the key competitive reactions within the ethanol-to-alkenes reaction network, namely C<sub>4</sub> alcohol dehydration and C-C chain growth, which dictate alkene product distributions. These findings indicate a feasible and promising method for tailoring alkene product distributions from ethanol upgrading, which is of notable significance to the generation of renewable middle distillates.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"344 ","pages":"Article 123648"},"PeriodicalIF":22.1,"publicationDate":"2023-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138816704","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}
Gang Qin , Xiaoyu Song , Qiang Chen , Wenjie He , Jia Yang , Yue Li , Yongcai Zhang , Jun Wang , Dionysios D. Dionysiou
{"title":"Novel durable and recyclable Cu@MoS2/polyacrylamide/copper alginate hydrogel photo-Fenton-like catalyst with enhanced and self-regenerable adsorption and degradation of high concentration tetracycline","authors":"Gang Qin , Xiaoyu Song , Qiang Chen , Wenjie He , Jia Yang , Yue Li , Yongcai Zhang , Jun Wang , Dionysios D. Dionysiou","doi":"10.1016/j.apcatb.2023.123640","DOIUrl":"10.1016/j.apcatb.2023.123640","url":null,"abstract":"<div><p>A durable and recyclable Cu@MoS<sub>2</sub><span><span>/polyacrylamide/copper alginate </span>nanocomposite double network (Cu@MoS</span><sub>2</sub>/PAAm/CA NCDN) hydrogel photo-Fenton-like catalyst was prepared for efficient removal of high concentration tetracycline (TC) in pharmaceutical wastewater. This hydrogel catalyst exhibits a remarkable synergistic effect between adsorption and catalytic degradation of TC. Consequently, this hydrogel catalyst shows a larger TC adsorption capacity of 122.2 mg g<sup>−1</sup> and a higher TC degradation efficiency of 90% (degradation amount = 70.2 mg g<sup>−1</sup>) at the TC concentration of 200 mg L<sup>−1</sup>, while the TC degradation efficiency by Cu@MoS<sub>2</sub> catalyst is only 19% (degradation amount = 38.2 mg g<sup>−1</sup>). This hydrogel catalyst can effectively remove high concentration TC under both light and dark conditions. Moreover, the tensile strength of Cu@MoS<sub>2</sub>/PAAm/CA NCDN hydrogel catalyst reaches an extraordinary 1.46 MPa and maintains 0.68 MPa after 15-day immersion in water, indicating high durability. In addition, the flexible hydrogel catalyst can keep good integrity after being deformed by stretching, bending, and knotting, etc., enabling its easy recovery. This investigation provides an innovative and versatile strategy to develop high-performance hydrogel catalysts for treating antibiotics-polluted water.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"344 ","pages":"Article 123640"},"PeriodicalIF":22.1,"publicationDate":"2023-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138988221","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}
Rasmus Lykke Mortensen , Hendrik-David Noack , Kim Pedersen , Maja A. Dunstan , Fabrice Wilhelm , Andrei Rogalev , Kasper S. Pedersen , Jerrik Mielby , Susanne Mossin
{"title":"Understanding the reversible and irreversible deactivation of methane oxidation catalysts","authors":"Rasmus Lykke Mortensen , Hendrik-David Noack , Kim Pedersen , Maja A. Dunstan , Fabrice Wilhelm , Andrei Rogalev , Kasper S. Pedersen , Jerrik Mielby , Susanne Mossin","doi":"10.1016/j.apcatb.2023.123646","DOIUrl":"10.1016/j.apcatb.2023.123646","url":null,"abstract":"<div><p>Catalytic oxidation is a promising technology for controlling methane emissions from natural gas engines, but fast and severe deactivation prevents implementation. We investigated a commercial Pd on alumina oxidation catalyst under realistic conditions and identified two deactivation phenomena: fast, reversible inhibition and slow, irreversible loss of active sites. The loss of active sites occurs only during methane conversion, fortunately a brief oxygen cut-off is enough to regenerate the catalyst. Both types of deactivation increase the reduction temperature of PdO. From 36 kinetic experiments we propose a simple kinetic model encompassing both types of deactivation. The inhibition is confirmed to be due to water coverage of the active sites whereas dispersion of Pd on the surface is the cause of the irreversible loss of active sites. The new insight shows a pathway toward designing more durable catalysts for complete methane oxidation.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"344 ","pages":"Article 123646"},"PeriodicalIF":22.1,"publicationDate":"2023-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0926337323012894/pdfft?md5=2754592b6a23989d6b5f6846c27fdf0c&pid=1-s2.0-S0926337323012894-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138816643","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}