Mengmeng Liu , Yan Zhang , Yucheng Xie , Guangxue Pan, Haiqun Cao, Sheng Ye
{"title":"TiO2 phase junction engineering for promoted interfacial adsorption and catalysis of imidacloprid insecticide","authors":"Mengmeng Liu , Yan Zhang , Yucheng Xie , Guangxue Pan, Haiqun Cao, Sheng Ye","doi":"10.1016/S1872-2067(25)64929-1","DOIUrl":"10.1016/S1872-2067(25)64929-1","url":null,"abstract":"<div><div>Imidacloprid (IMI) is one of the best-selling insecticides worldwide in modern agricultural pest control. However, the extensive and persistent application of IMI raises concerns regarding ecological disruption and health hazards. Although semiconductor photocatalysis offers a promising remediation pathway, the interplay between catalyst structure, degradation selectivity, and environmental safety remains poorly understood. Herein, we report an anatase/rutile TiO<sub>2</sub> phase junction (A/R-TiO<sub>2</sub>) for photocatalytic IMI remediation. The A/R-TiO<sub>2</sub> exhibits 11.5-fold and 27.7-fold higher than those of A-TiO<sub>2</sub> and R-TiO<sub>2</sub> in rate constant, with a high mineralization rate of 87.6%. It is found that toxic intermediates during the degradation process of A-TiO<sub>2</sub> and R-TiO<sub>2</sub> are generated, while the final degradation products of A/R-TiO<sub>2</sub> show non-toxicity, confirmed by high performance liquid chromatography-mass spectrometry analysis and biological assessments. Density functional theory calculations demonstrate that compared with single-site adsorption of IMI on A-TiO<sub>2</sub> and R-TiO<sub>2</sub>, the interfacial dual-site adsorption on A/R-TiO<sub>2</sub> strengthens the adsorption energy of IMI, accelerates charge separation, and promotes catalytic degradation. These findings underscore the need to establish a structure-function-toxicity framework that redefines photocatalyst design around both kinetic performance and environmental safety.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"84 ","pages":"Pages 359-367"},"PeriodicalIF":17.7,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826641","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}
Yun Xing , Lei Liu , Wen-Jing Kong , Jun-Tai Tian , Peng Liu , Chen Yang , Ming-Li Fu , Dai-Qi Ye
{"title":"Ce-activated metallic foam carriers for efficient butyl acetate oxidation: Dual roles of intrinsic redox cycling and interfacial electron transfer","authors":"Yun Xing , Lei Liu , Wen-Jing Kong , Jun-Tai Tian , Peng Liu , Chen Yang , Ming-Li Fu , Dai-Qi Ye","doi":"10.1016/S1872-2067(26)64994-7","DOIUrl":"10.1016/S1872-2067(26)64994-7","url":null,"abstract":"<div><div>Oxygenated volatile organic compounds (OVOCs) exemplified by butyl acetate, which posed severe environmental and health risks due to their low odor threshold, substantial industrial emissions, and detrimental ecological effects. The efficient abatement of OVOCs was not only imperative for air quality improvement but also aligned with the core principles of green chemistry by minimizing the release of hazardous volatiles and reducing energy consumption. There was an urgent need to develop highly efficient catalytic technologies to mitigate the persistent threat these compounds present to atmospheric environments and public health. In this study, cerium (Ce)-based monolithic catalysts synthesized by in situ growth method were developed for practical catalytic applications and demonstrated enhanced active species loading capacity. The introduction of Ce leveraged the inherent high oxygen storage capacity of CeO<sub>2</sub> to enhance reactant activation and oxidation. Meanwhile, Ce species activate the alloy on the metallic foam support, facilitating electron transfer and promoting redox cycles between Ce<sup>4+</sup>/Ce<sup>3+</sup>, Co<sup>3+</sup>/Co<sup>2+</sup>, and Ni<sup>2+</sup>/Ni<sup>3+</sup>. This process concurrently induced additional oxygen vacancies formation. Thus, the Ce/Co-Ni foam catalyst exhibited exceptional removal efficiency exceeding 99% at 230 °C. Furthermore, it maintained removal performance above 80% under challenging conditions, including prolonged operation and the presence of 8 vol% H<sub>2</sub>O. This study revealed that the foam substrate within the monolithic catalyst served not only as structural support but also functioned as an active component, significantly influencing the overall catalytic activity. These findings provided a novel strategy for designing high-performance monolithic foam catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"84 ","pages":"Pages 390-400"},"PeriodicalIF":17.7,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826695","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}
Xintong Lv , Zhengchang Wei , Xin Deng , Yuchao Chai , Guangjun Wu , Landong Li
{"title":"Isolated Pt sites anchored by skeletal Fe in MFI zeolite nanosheets towards productive propane dehydrogenation","authors":"Xintong Lv , Zhengchang Wei , Xin Deng , Yuchao Chai , Guangjun Wu , Landong Li","doi":"10.1016/S1872-2067(26)65003-6","DOIUrl":"10.1016/S1872-2067(26)65003-6","url":null,"abstract":"<div><div>The development of effective alkane dehydrogenation catalysts is essential to produce olefins from abundant shale gas. Commercial Pt-based propane dehydrogenation catalysts suffer from deactivation due to sintering and coke deposition, highlighting the need for substantial improvements in thermal stability and production efficiency. Herein, we present a facile one-pot strategy to create atomically dispersed bimetallic Pt-O-Fe motifs encapsulated within MFI zeolite nanosheet, serving as highly active and stable sites for propane dehydrogenation. Comprehensive characterization results reveal that the skeletal Fe (III) species in MFI zeolite act as anchoring sites, thereby stabilizing atomically dispersed Pt species through the unique linkages of ≡Si-O-Fe-O-Pt. The optimized 0.3Pt2Fe@NS catalyst, featuring high skeletal Fe content, low Pt loading, and ideal synergetic effect of Pt-Fe endowed by the suitable Pt-to-Fe ratio, achieves a propylene productivity of 48.0 mmol C<sub>3</sub>H<sub>6</sub>·g<sub>cat</sub><sup>−1</sup>·h<sup>−1</sup> with >95% selectivity at 550 °C for 30 h without performance degradation. The 0.3Pt2Fe@NS catalyst also exhibits complete regenerability under harsh cycling conditions, establishing a new structure-performance paradigm for the design of industrial PDH catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"84 ","pages":"Pages 61-73"},"PeriodicalIF":17.7,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826892","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}
Wenning Liu , Li An , Jinming Wang , Ruyue Li , Jie Mu , Yongde Long , Dan Qu , Yichang Liu , Yuxiang Hu , Xiayan Wang , Ning Jiang , Zaicheng Sun
{"title":"Group IIIA metals-induced p-d orbital hybridization enhances the oxygen reduction performance of Pd based metallene in zinc-air batteries","authors":"Wenning Liu , Li An , Jinming Wang , Ruyue Li , Jie Mu , Yongde Long , Dan Qu , Yichang Liu , Yuxiang Hu , Xiayan Wang , Ning Jiang , Zaicheng Sun","doi":"10.1016/S1872-2067(26)64964-9","DOIUrl":"10.1016/S1872-2067(26)64964-9","url":null,"abstract":"<div><div><em>p-d</em> orbital hybridization offers a powerful strategy to optimize oxygen adsorption energies and accelerate the oxygen reduction reaction (ORR) in zinc-air batteries (ZABs). Here, we introduce Group IIIA elements (Al, Ga, In) into PdPtMo metallenes to systematically tune <em>p-d</em> orbital interactions. Among them, Ga exhibits the smallest atomic radius mismatch and optimal orbital energy alignment, and the enhanced <em>p-d</em> orbital hybridization in PdPtMoGa metallenes promotes electron transfer. The PdPtMoGa metallene/C catalyst achieves an exceptionally high mass activity of 6.07 A mg<sup>−1</sup><sub>Pt</sub> at 0.9 V <em>vs</em>. RHE and a half-wave potential of 0.94 V, surpassing commercial Pt/C. Density functional theory calculations, X-ray absorption spectroscopy, <em>in-situ</em> Fourier-transform infrared spectroscopy, and other characterizations reveal that the strong <em>p-d</em> orbital hybridization induced by Ga coordination with Pd in PdPtMoGa metallenes lowers the <em>d</em>-band center and weakens the adsorption of oxygen intermediates. Remarkably, the catalyst retains stability over 30,000 cycles. When deployed in ZABs, PdPtMoGa metallene/C achieves a peak power density of 207.2 mW cm<sup>−2</sup> and stable operation exceeding 180 h. Overall, this study presents a rational design strategy for high-activity and durable Pd-based electrocatalysts and elucidates the specific roles of Group IIIA elements in modulating <em>p-d</em> orbital hybridization.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"84 ","pages":"Pages 144-158"},"PeriodicalIF":17.7,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826413","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}
Jingyao Wu , Yujing Lv , Qiang Zhao , Shuo Wang , Ying Wang , Na Wen , Zhengxin Ding , Zizhong Zhang , Jinlin Long
{"title":"Electron-proton duet in covalent organic frameworks for efficient direct oxygen reduction to hydrogen peroxide","authors":"Jingyao Wu , Yujing Lv , Qiang Zhao , Shuo Wang , Ying Wang , Na Wen , Zhengxin Ding , Zizhong Zhang , Jinlin Long","doi":"10.1016/S1872-2067(26)64990-X","DOIUrl":"10.1016/S1872-2067(26)64990-X","url":null,"abstract":"<div><div>The proton adsorption capacity, equally critical as photogenerated electron accumulation at active sites, jointly governs efficient hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production through the one-step 2e<sup>−</sup> direct oxygen reduction reaction (ORR) in covalent organic frameworks (COFs). Herein, TPNN-COF incorporates precisely tailored triazine and pyridine nitrogen centers, establishing an optimal proton harvesting interface that enables direct proton capture from aqueous phase to catalytic ORR sites. Concurrently, the complementary electronic effects of triazine and pyridine nitrogen moieties collectively optimize the donor-acceptor (D-A) architecture in TPNN-COF, thereby significantly improving photogenerated charge separation. This dual optimization of proton and electron dynamics creates a harmonious interplay that fundamentally restructures the reaction pathway from conventional two-step 1e<sup>−</sup> indirect mechanisms to efficient one-step 2e<sup>−</sup> direct ORR processes. The resulting photocatalytic system achieves an exceptional hydrogen peroxide production of 3584.9 μmol g<sup>−1</sup> h<sup>−1</sup> under visible light irradiation in sacrificial-agent-free pure aqueous media under air, representing 4.1-fold and 3.4-fold improvements over pyridine-deficient TPNB-COF and triazine-deficient TPBN-COF respectively, while demonstrating an impressive 4.1% apparent quantum yield at 420 nm. These insights provide a novel strategy for constructing efficient direct ORR reaction sites while advancing the mechanistic understanding of ORR processes in advanced photocatalytic systems for sustainable chemical synthesis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"84 ","pages":"Pages 288-300"},"PeriodicalIF":17.7,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826636","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}
Jian Li , Zhenfa Wu , Xinru Zhang , Tongan Yan , Jin Luo , Wenjuan Xue , Zhaolin Lv , Hongliang Huang , Chongli Zhong
{"title":"Dynamic coordination transformation from single-to dual-metal sites in MOFs for cascaded photoreforming of plastics into CO","authors":"Jian Li , Zhenfa Wu , Xinru Zhang , Tongan Yan , Jin Luo , Wenjuan Xue , Zhaolin Lv , Hongliang Huang , Chongli Zhong","doi":"10.1016/S1872-2067(26)65013-9","DOIUrl":"10.1016/S1872-2067(26)65013-9","url":null,"abstract":"<div><div>Building on the success of catalytic single-metal sites (SMSs) in various model reaction systems, dual-metal sites (DMSs) could provide further breakthrough on catalysing complex reactions especially for those involving multiple cascading steps. Specifically, photocatalytic waste plastic conversion requires bond cleavage into small molecules followed by site-dependent transformations, where DMSs photocatalysts can, in principle, be highly active and selective through efficient charge separation and dual-site synergy. However, related studies remain rare since difficulty on efficient waste plastic photodegradation usually hinders subsequent catalytic conversion. Herein, we report for the first time that dual-metal sites are developed in a two-dimensional metal-organic framework (MOF) (Cu<sub>2</sub>-DMSs/MOF) derived from single-metal sites in bulk MOF (Cu<sub>1</sub>-SMSs/MOF) via dynamic coordination-driven transformation. The Cu<sub>2</sub>-DMSs/MOF catalyst exhibits enhanced photocatalytic performance without sacrificial agents, catalysing the cascading polyethylene-to-CO<sub>2</sub> and CO<sub>2</sub>-to-CO reactions in one step. The polyethylene-to-CO<sub>2</sub> degradation rate is 2.32 mmol·g<sup>−1</sup>·h<sup>−1</sup> and the subsequent CO<sub>2</sub>-to-CO conversion proceeds at 0.29 mmol·g<sup>−1</sup>·h<sup>−1</sup> with 100% selectivity, representing an order-of-magnitude enhancement compared with previous reports. The *O<sub>2</sub><sup>−</sup> and *OH radicals formed from O<sub>2</sub> and H<sub>2</sub>O oxidative cleave C–C and C–H bonds in polyethylene to CO<sub>2</sub>, which is subsequentially selective reduced to CO via multi-electron proton-coupling. This work offers a conceptual advance in designing dual-metal site catalysts, opening new avenues for cascading photocatalytic conversion of white pollution into valuable chemicals.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"84 ","pages":"Pages 314-323"},"PeriodicalIF":17.7,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826642","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}
Ruiwen Hu , Zhiyong Guo , Xiaogang Peng , Xiaoqi Shi, Yuben Qiao, Qian Li, Chenghua Gao, Aitao Li
{"title":"Synergistic integration of ancestral sequence reconstruction and rational design empowers unspecific peroxygenase for efficient steroid core oxyfunctionalization","authors":"Ruiwen Hu , Zhiyong Guo , Xiaogang Peng , Xiaoqi Shi, Yuben Qiao, Qian Li, Chenghua Gao, Aitao Li","doi":"10.1016/S1872-2067(26)64991-1","DOIUrl":"10.1016/S1872-2067(26)64991-1","url":null,"abstract":"<div><div>Unspecific peroxygenases (UPOs) are versatile biocatalysts for selective oxyfunctionalization, yet their use in steroid core hydroxylation remains underdeveloped. Although <em>Cgl</em>UPO is the best-studied steroid-hydroxylating UPO, its inefficiency and tendency to form unwanted epoxides limit its practicality. To overcome this, we employed ancestral sequence reconstruction (ASR) to obtain ancestral UPO N1 that exhibited 3-fold higher expression than modern counterparts <em>Cgl</em>UPO and demonstrated moderate regioselectivity (63%) for 11<em>β</em>-hydroxylation of estra-4,9-diene-3,17-dione (<strong>1</strong>). Guided by molecular dynamics simulations, rational mutagenesis of key substrate-binding residues generated the variant N1-F83G/L232V. This variant achieved a 36-fold increase in catalytic activity with near-complete 11<em>β</em>-regioselectivity (99%). Mechanistic study revealed that L232V reduces steric hindrance near the active site, while F83G eliminates a mispositioned hydrophobic anchor—challenging the paradigm that hydrophobic interactions always benefit catalysis. Substrate scope studies confimred the broad applicability of this variant, yielding different hydroxylation patterns (11<em>β</em>-, 16<em>α</em>-, 6<em>β</em>-) depending on steroids tested. Gram-scale synthesis afforded isolated yields of 40~86% for different hydroxylated steriods, which serve as pivotal intermediates for synthesizing desogestrel, estriol, and exemestane. Overall, this work advances the steroid biocatalysis toolbox, demonstrates how integraing ASR with rational engineering solves UPO limitations, and establishes UPOs as industrially viable catalysts for steroid pharmaceutical synthesis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"84 ","pages":"Pages 417-427"},"PeriodicalIF":17.7,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826643","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}
Peixin Zhu , Mengyao Xiao , Xixi Chen , Jingsong Luo , Zhong Fang , Long Chen , Huinan Zhao , Chun He , Shuanghong Tian
{"title":"Microstructure modulation of α-MnO2 via mild urea-induced phase transition for enhanced catalytic ozonation of emerging contaminants","authors":"Peixin Zhu , Mengyao Xiao , Xixi Chen , Jingsong Luo , Zhong Fang , Long Chen , Huinan Zhao , Chun He , Shuanghong Tian","doi":"10.1016/S1872-2067(25)64889-3","DOIUrl":"10.1016/S1872-2067(25)64889-3","url":null,"abstract":"<div><div>While facet engineering and heterostructure construction are recognized as effective strategies for enhancing catalytic performance through defect creation, their integration remains scarce and challenging. This study develops a mild urea-assisted thermal strategy to construct an oxygen vacancy (OV)-rich <em>α</em>-MnO<sub>2</sub>(310)/Mn<sub>3</sub>O<sub>4</sub> heterojunction (Mn400-0.125U), comprising 48.6% <em>α</em>-MnO<sub>2</sub> with preferentially exposed (310) facets and 51.4% Mn<sub>3</sub>O<sub>4</sub>. The low OV formation energy on (310) facets coupled with heterojunction interfaces effects leads to a high OV concentration. Mn400-0.125U demonstrated exceptional catalytic ozonation performance, achieving a sulfamethoxazole degradation rate constant (7.7×10<sup>−2</sup> min<sup>−1</sup>), which is 1.8-, 1.6-, and 3.3-fold higher than those of <em>α</em>-MnO<sub>2</sub>, Mn<sub>3</sub>O<sub>4</sub>, and single ozonation, respectively. Operational advantages include ultralow catalyst dosage (0.1 g/L), broad pH adaptability (3.5–10.5), and remarkable resilience against aqueous matrix interference (≤ 12.4% efficiency loss). Both experimental and theoretical calculations demonstrate that the abundant OVs, combined with the proper hydrophilicity of Mn400-0.125U, synergistically trigger barrier-free activation and decomposition of ozone, subsequently generating a series of reactive species via chain reactions. A hybrid oxidation regime was identified where the non-radical pathway mediated by electron-transfer, O* (surface oxygen atoms), and <sup>1</sup>O<sub>2</sub> predominates over radical pathways (•O<sub>2</sub><sup>−</sup>/•OH). This work establishes a facile coupled modulation protocol for creating defect-rich manganese oxides applied in catalytic ozonation of emerging contaminants.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"84 ","pages":"Pages 175-188"},"PeriodicalIF":17.7,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826524","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}
Chengyang Sun , Haochen Zhang , Xiaohui Liu, Yanqin Wang
{"title":"Oxygen vacancy promoted C–H activation enhancing hydrogenolysis of polyethylene plastics over Ru/CeO2 catalyst","authors":"Chengyang Sun , Haochen Zhang , Xiaohui Liu, Yanqin Wang","doi":"10.1016/S1872-2067(25)64897-2","DOIUrl":"10.1016/S1872-2067(25)64897-2","url":null,"abstract":"<div><div>Catalytic hydrogenolysis offers a promising route for plastic waste upcycling. Herein, we demonstrate that oxygen vacancies (O<sub>V</sub>) in CeO<sub>2</sub> supports dramatically enhanced this process. Reduction-engineered Ru/CeO<sub>2</sub>-NH<sub>3</sub>-800 exhibits 40% higher activity at 800 °C than untreated counterparts. Comprehensive characterization revealed unchanged Ru metal sites after treatment, but significantly increased oxygen vacancy content in the CeO<sub>2</sub> support. Isotopic C<sub>6</sub>–D<sub>2</sub> temperature-programmed surface reaction studies revealed that higher O<sub>V</sub> concentrations correlate with lower C–H bond activation temperatures, directly aligning with observed activity trends. We propose a novel Ru–Ce interfacial mechanism: O<sub>V</sub>-adjacent Ce<sup>3+</sup>–O sites activate C–H bonds to form *RCCR* intermediates, while dual Ru sites cleave C–C bonds via C–Ru coordination. This work establishes an O<sub>V</sub>-driven structure-activity relationship for the first time and reveals support-mediated C–H activation as crucial for advanced catalyst design.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"84 ","pages":"Pages 337-346"},"PeriodicalIF":17.7,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826639","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}
Jingjing Shi , Yanju Lu , Kui Wang , Zupeng Chen , Junming Xu , Jianchun Jiang
{"title":"Highly efficient electrocatalytic reductive cleavage of lignin model compounds over Ru@Bi/N-C: Interfacial and defect effects","authors":"Jingjing Shi , Yanju Lu , Kui Wang , Zupeng Chen , Junming Xu , Jianchun Jiang","doi":"10.1016/S1872-2067(26)65005-X","DOIUrl":"10.1016/S1872-2067(26)65005-X","url":null,"abstract":"<div><div>Understanding and regulating the substrate adsorption behavior and hydrogen species (H<sub>spe</sub>) migration channels are crucial for achieving efficient lignin electrocatalytic hydrogenation (ECH). This effective Bi-Ru interface and adjacent N-defect sites were constructed on Ru@Bi/N-C catalyst, thereby controllably modulating the blocking and exposure of substrate adsorption sites while establishing ideal H<sub>spe</sub> migration pathways. By introducing heteropolyacid (HPW) and hexafluoroisopropanol (HFIP) electrolyte, the conversion of 2-phenoxy-1-phenylethanol attained 93.64%, with Faraday efficiency (FE) of 91.92%. Moreover, the high hydrogenation deoxygenation efficiency (> 90%) was also obtained for phenolic monomers, demonstrating superior performance compared to most advanced electrocatalytic systems. Synchrotron radiation, <em>in-situ</em> Raman, and density functional theory calculations have demonstrated that the Bi-Ru interface obstructed the strong substrates adsorption on the Ru crystal surface, thereby facilitating the adsorption-activation and rapid desorption at N-defect sites. The blocking effect of Bi-Ru interface inhibited the hydrogen evolution reaction while promoting the spillover of adsorbed hydrogen (H<sub>ads</sub>) to enable efficient ECH. Additionally, HPW mediated electron transfer could supply abundant H<sub>ads</sub>, whereas polar HFIP promoted the protonation of substrate hydroxyl. This research developed a universal strategy for creating an exquisite catalytic network and establishing an optimized electrolyte microenvironment, providing significant insights for the development of highly efficient lignin ECH systems.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"84 ","pages":"Pages 401-416"},"PeriodicalIF":17.7,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826696","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}