Chinese Journal of Catalysis最新文献_第2页

Atomic orbitals modulated dual functional bimetallic phosphides derived from MOF on MOF structure for boosting high efficient overall water splitting 在 MOF 结构上衍生 MOF 的原子轨道调制双功能双金属磷化物，促进高效整体水分离

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-10-01 DOI: 10.1016/S1872-2067(24)60124-5

Bohan An , Weilong Liu , Jipeng Dong , Ning Li , Yangqin Gao , Lei Ge

{"title":"Atomic orbitals modulated dual functional bimetallic phosphides derived from MOF on MOF structure for boosting high efficient overall water splitting","authors":"Bohan An , Weilong Liu , Jipeng Dong , Ning Li , Yangqin Gao , Lei Ge","doi":"10.1016/S1872-2067(24)60124-5","DOIUrl":"10.1016/S1872-2067(24)60124-5","url":null,"abstract":"<div><div>The electronic modulation characteristics of efficient metal phosphide electrocatalysts can be utilized to tune the performance of oxygen evolution reaction (OER). However, improving the overall water splitting performance remains a challenging task. By building metal organic framework (MOF) on MOF heterostructures, an efficient strategy for controlling the electrical structure of MOFs was presented in this study. ZIF-67 was in-situ synthesized on MIL-88 (Fe) using a two-step self-assembly method, followed by low-temperature phosphorization to ultimately synthesize FeP-CoP3 bimetallic phosphides. By combining atomic orbital theory and theoretical calculations (density functional theory), the results reveal the successful modulation of electronic orbitals in FeP-CoP3 bimetallic phosphides, which are synthesized from MOF on MOF structure. The synergistic impact of the metal center Co species and the phase conjugation of both kinds of MOFs are responsible for this regulatory phenomenon. Therefore, the catalyst demonstrates excellent properties, demonstrating HER 81 mV (η10) in a 1.0 mol L−1 KOH solution and OER 239 mV (η50) low overpotentials. The FeP-CoP3 linked dual electrode alkaline batteries, which are bifunctional electrocatalysts, have a good electrocatalytic ability and may last for 50 h. They require just 1.49 V (η50) for total water breakdown. Through this technique, the electrical structure of electrocatalysts may be altered to increase catalytic activity.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"65 ","pages":"Pages 113-125"},"PeriodicalIF":15.7,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142527235","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}

引用次数: 0

Interfacial coordination bonds accelerate charge separation for unprecedented hydrogen evolution over S-scheme heterojunction 表面配位键加速电荷分离，使 S 型异质结实现前所未有的氢演化

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-10-01 DOI: 10.1016/S1872-2067(24)60108-7

Chunxue Li , Hao Lu , Guixiang Ding , Tianyi Ma , Shiyong Liu , Li Zhang , Guangfu Liao

{"title":"Interfacial coordination bonds accelerate charge separation for unprecedented hydrogen evolution over S-scheme heterojunction","authors":"Chunxue Li , Hao Lu , Guixiang Ding , Tianyi Ma , Shiyong Liu , Li Zhang , Guangfu Liao","doi":"10.1016/S1872-2067(24)60108-7","DOIUrl":"10.1016/S1872-2067(24)60108-7","url":null,"abstract":"<div><div>Inspired by natural photosynthesis, fabricating high-performance S-scheme heterojunction is regarded as a successful tactic to address energy and environmental issues. Herein, NH2-MIL-125(Ti)/Zn0.5Cd0.5S/NiS (NMT/ZCS/NiS) S-scheme heterojunction with interfacial coordination bonds is successfully synthesized through in-situ solvothermal strategy. Notably, the optimal NMT/ZCS/NiS S-scheme heterojunction exhibits comparable photocatalytic H2 evolution (PHE) rate of about 14876.7 μmol h−1 g−1 with apparent quantum yield of 24.2% at 420 nm, which is significantly higher than that of recently reported MOFs-based photocatalysts. The interfacial coordination bonds (Zn–N, Cd–N, and Ni–N bonds) accelerate the separation and transfer of photogenerated charges, and the NiS as cocatalyst can provide more catalytically active sites, which synergistically improve the photocatalytic performance. Moreover, theoretical calculation results display that the construction of NMT/ZCS/NiS S-scheme heterojunction also optimize the binding energy of active site-adsorbed hydrogen atoms to enable fast adsorption and desorption. Photoassisted Kelvin probe force microscopy, in-situ irradiation X-ray photoelectron spectroscopy, femtosecond transient absorption spectroscopy, and theoretical calculations provide sufficient evidence of the S-scheme charge migration mechanism. This work offers unique viewpoints for simultaneously accelerating the charge dynamics and optimizing the binding strength between the active sites and hydrogen adsorbates over S-scheme heterojunction.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"65 ","pages":"Pages 174-184"},"PeriodicalIF":15.7,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142527159","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}

引用次数: 0

Mechanism study on the influence of surface properties on the synthesis of dimethyl carbonate from CO2 and methanol over ceria catalysts 表面性质对铈催化剂以二氧化碳和甲醇为原料合成碳酸二甲酯的影响机理研究

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-10-01 DOI: 10.1016/S1872-2067(24)60091-4

Lei Dong , Shengjie Zhu , Yangyang Yuan , Xiaomin Zhang , Xiaowei Zhao , Yanping Chen , Lei Xu

{"title":"Mechanism study on the influence of surface properties on the synthesis of dimethyl carbonate from CO2 and methanol over ceria catalysts","authors":"Lei Dong , Shengjie Zhu , Yangyang Yuan , Xiaomin Zhang , Xiaowei Zhao , Yanping Chen , Lei Xu","doi":"10.1016/S1872-2067(24)60091-4","DOIUrl":"10.1016/S1872-2067(24)60091-4","url":null,"abstract":"<div><div>The direct synthesis of dimethyl carbonate (DMC) from CO2 and methanol has attracted much attention as an environmentally benign and alternative route for conventional routes. Herein, a series of cerium oxide catalysts with various textural features and surface properties were prepared by the one-pot synthesis method for the direct DMC synthesis from CO2 and methanol, and the structure-performance relationship was investigated in detail. Characterization results revealed that both of surface acid-base properties and the oxygen vacancies contents decreased with the rising crystallinity at increasingly higher calcination temperature accompanied by an unexpectedly volcano-shaped trend of DMC yield observed on the catalysts. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) studies indicated that the adsorption rate of methanol is slower than that of CO2 and the methanol activation state largely influences the formation of key intermediate. Although the enhanced surface acidity-basicity and oxygen vacancies brought by low-temperature calcination could facilitate the activation of CO2, the presence of excess strongly basic sites on low-crystallinity sample was detrimental to DMC synthesis due to the preferred formation of unreactive mono/polydentate carbonates as well as the further impediment of methanol activation. Moreover, with the use of 2-cyanopyridine as a dehydration reagent, the DMC synthesis was found to be both influenced by the promotion from the rapid in situ removal of water and the inhibition from the competitive adsorption of hydration products on the same active sites.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"65 ","pages":"Pages 138-152"},"PeriodicalIF":15.7,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142527156","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}

引用次数: 0

Mild polarization electric field in ultra-thin BN-Fe-graphene sandwich structure for efficient nitrogen reduction 超薄 BN-Fe-Graphene 夹层结构中的温和极化电场可实现高效氮还原

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-10-01 DOI: 10.1016/S1872-2067(24)60114-2

Ziyuan Xiu , Wei Mu , Xin Zhou , Xiaojun Han

{"title":"Mild polarization electric field in ultra-thin BN-Fe-graphene sandwich structure for efficient nitrogen reduction","authors":"Ziyuan Xiu , Wei Mu , Xin Zhou , Xiaojun Han","doi":"10.1016/S1872-2067(24)60114-2","DOIUrl":"10.1016/S1872-2067(24)60114-2","url":null,"abstract":"<div><div>The electrocatalytic N2 reduction reaction (NRR) is expected to supersede the traditional Haber-Bosch technology for NH3 production under ambient conditions. The activity and selectivity of electrochemical NRR are restricted to a strong polarized electric field induced by the catalyst, correct electron transfer direction, and electron tunneling distance between bare electrode and active sites. By coupling the chemical vapor deposition method with the poly(methyl methacylate)-transfer method, an ultrathin sandwich catalyst, i.e., Fe atoms (polarized electric field layer) sandwiched between ultrathin (within electron tunneling distance) BN (catalyst layer) and graphene film (conducting layer), is fabricated for electrocatalytic NRR. The sandwich catalyst not only controls the transfer of electrons to the BN surface in the correct direction under applied voltage but also suppresses hydrogen evolution reaction by constructing a neutral polarization electric field without metal exposure. The sandwich electrocatalyst NRR system achieve NH3 yield of 8.9 μg h−1 cm−2 and Faradaic Efficiency of 21.7%. The N2 adsorption, activation, and polarization electric field changes of three sandwich catalysts (BN-Fe-G, BN-Fe-BN, and G-Fe-G) during the electrocatalytic NRR are investigated by experiments and density functional theory simulations. Driven by applied voltage, the neutral polarized electric field induced by BN-Fe-G leads to the high activity of electrocatalytic NRR.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"65 ","pages":"Pages 126-137"},"PeriodicalIF":15.7,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142527243","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}

引用次数: 0

Efficient electrocatalytic urea synthesis from CO2 and nitrate over the scale-up produced FeNi alloy-decorated nanoporous carbon 在规模化生产的铁镍合金装饰纳米多孔碳上高效电催化二氧化碳和硝酸盐合成尿素

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-10-01 DOI: 10.1016/S1872-2067(24)60111-7

Zuo-Shu Sun , Xue-Yan Xiang , Qiu-Ping Zhao , Zhao Tang , Shi-Yi Jiang , Tong-Bu Lu , Zhi-Ming Zhang , Baifan Wang , Hua-Qing Yin

{"title":"Efficient electrocatalytic urea synthesis from CO2 and nitrate over the scale-up produced FeNi alloy-decorated nanoporous carbon","authors":"Zuo-Shu Sun , Xue-Yan Xiang , Qiu-Ping Zhao , Zhao Tang , Shi-Yi Jiang , Tong-Bu Lu , Zhi-Ming Zhang , Baifan Wang , Hua-Qing Yin","doi":"10.1016/S1872-2067(24)60111-7","DOIUrl":"10.1016/S1872-2067(24)60111-7","url":null,"abstract":"<div><div>Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis, but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging. Herein, we developed a simple method for the preparation of a series of FeNi-alloy-based catalysts, named FeNi@nC-T (n represents the content of nanoporous carbon as 1, 3, 5, 7 or 9 g and T = 900, 950, 1000 or 1100 °C), for highly performed urea synthesis via NO3− and CO2 co-reduction. The FeNi@7C-1000 achieved a high urea yield of 1041.33 mmol h−1 gFeNi−1 with a Faradaic efficiency of 15.56% at –1.2 V vs. RHE. Moreover, the scale-up synthesized FeNi@7C-950-S (over 140 g per batch) was achieved with its high catalytic performance and high stability maintained. Mechanism investigation illuminated that the Ni and Fe sites catalyze and stabilize the key *CO and *N intermediates and minimize the C–N coupling reaction barriers for highly efficient urea synthesis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"65 ","pages":"Pages 153-162"},"PeriodicalIF":15.7,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142527157","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}

引用次数: 0

Chalcogen heteroatoms doped nickel-nitrogen-carbon single-atom catalysts with asymmetric coordination for efficient electrochemical CO2 reduction 掺杂查耳根杂原子的镍-氮-碳单原子不对称配位催化剂用于高效的二氧化碳电化学还原反应

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-09-01 DOI: 10.1016/S1872-2067(24)60103-8

Jialin Wang , Kaini Zhang , Ta Thi Thuy Nga , Yiqing Wang , Yuchuan Shi , Daixing Wei , Chung-Li Dong , Shaohua Shen

{"title":"Chalcogen heteroatoms doped nickel-nitrogen-carbon single-atom catalysts with asymmetric coordination for efficient electrochemical CO2 reduction","authors":"Jialin Wang , Kaini Zhang , Ta Thi Thuy Nga , Yiqing Wang , Yuchuan Shi , Daixing Wei , Chung-Li Dong , Shaohua Shen","doi":"10.1016/S1872-2067(24)60103-8","DOIUrl":"10.1016/S1872-2067(24)60103-8","url":null,"abstract":"<div>The electronic configuration of central metal atoms in single-atom catalysts (SACs) is pivotal in electrochemical CO2 reduction reaction (eCO2RR). Herein, chalcogen heteroatoms (e.g., S, Se, and Te) were incorporated into the symmetric nickel-nitrogen-carbon (Ni-N4-C) configuration to obtain Ni-X-N3-C (X: S, Se, and Te) SACs with asymmetric coordination presented for central Ni atoms. Among these obtained Ni-X-N3-C (X: S, Se, and Te) SACs, Ni-Se-N3-C exhibited superior eCO2RR activity, with CO selectivity reaching ~98% at −0.70 V versus reversible hydrogen electrode (RHE). The Zn-CO2 battery integrated with Ni-Se-N3-C as cathode and Zn foil as anode achieved a peak power density of 1.82 mW cm–2 and maintained remarkable rechargeable stability over 20 h. In-situ spectral investigations and theoretical calculations demonstrated that the chalcogen heteroatoms doped into the Ni-N4-C configuration would break coordination symmetry and trigger charge redistribution, and then regulate the intermediate behaviors and thermodynamic reaction pathways for eCO2RR. Especially, for Ni-Se-N3-C, the introduced Se atoms could significantly raise the d-band center of central Ni atoms and thus remarkably lower the energy barrier for the rate-determining step of *COOH formation, contributing to the promising eCO2RR performance for high selectivity CO production by competing with hydrogen evolution reaction.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"64 ","pages":"Pages 54-65"},"PeriodicalIF":15.7,"publicationDate":"2024-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142122659","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}

引用次数: 0

Poly(ethylenimine)-assisted synthesis of hollow carbon spheres comprising multi-sized Ni species for CO2 electroreduction 聚（乙烯亚胺）辅助合成包含多尺寸镍物种的空心碳球，用于二氧化碳电还原

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-09-01 DOI: 10.1016/S1872-2067(24)60087-2

Kaining Li , Yasutaka Kuwahara , Hiromi Yamashita

{"title":"Poly(ethylenimine)-assisted synthesis of hollow carbon spheres comprising multi-sized Ni species for CO2 electroreduction","authors":"Kaining Li , Yasutaka Kuwahara , Hiromi Yamashita","doi":"10.1016/S1872-2067(24)60087-2","DOIUrl":"10.1016/S1872-2067(24)60087-2","url":null,"abstract":"<div>Electrochemical CO2 reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy conversion. The development of efficient catalysts with high conductivity and readily accessible active sites for CO2 electroreduction remains challenging yet indispensable. In this work, a reliable poly(ethyleneimine) (PEI)-assisted strategy is developed to prepare a hollow carbon nanocomposite comprising a single-site Ni-modified carbon shell and confined Ni nanoparticles (NPs) (denoted as Ni@NHCS), where PEI not only functions as a mediator to induce the highly dispersed growth of Ni NPs within hollow carbon spheres, but also as a nitrogen precursor to construct highly active atomically-dispersed Ni-Nx sites. Benefiting from the unique structural properties of Ni@NHCS, the aggregation and exposure of Ni NPs can be effectively prevented, while the accessibility of abundant catalytically active Ni-Nx sites can be ensured. As a result, Ni@NHCS exhibits a high CO partial current density of 26.9 mA cm–2 and a Faradaic efficiency of 93.0% at −1.0 V vs. RHE, outperforming those of its PEI-free analog. Apart from the excellent activity and selectivity, the shell confinement effect of the hollow carbon sphere endows this catalyst with long-term stability. The findings here are anticipated to help understand the structure-activity relationship in Ni-based carbon catalyst systems for electrocatalytic CO2 reduction. Furthermore, the PEI-assisted synthetic concept is potentially applicable to the preparation of high-performance metal-based nanoconfined materials tailored for diverse energy conversion applications and beyond.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"64 ","pages":"Pages 66-76"},"PeriodicalIF":15.7,"publicationDate":"2024-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142122660","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}

引用次数: 0

Single-atom modified graphene cocatalyst for enhanced photocatalytic CO2 reduction on halide perovskite 单原子修饰石墨烯协同催化剂用于增强卤化物过氧化物上的二氧化碳光催化还原能力

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-09-01 DOI: 10.1016/S1872-2067(24)60081-1

Hui Fu, Jin Tian, Qianqian Zhang, Zhaoke Zheng, Hefeng Cheng, Yuanyuan Liu, Baibiao Huang, Peng Wang

{"title":"Single-atom modified graphene cocatalyst for enhanced photocatalytic CO2 reduction on halide perovskite","authors":"Hui Fu, Jin Tian, Qianqian Zhang, Zhaoke Zheng, Hefeng Cheng, Yuanyuan Liu, Baibiao Huang, Peng Wang","doi":"10.1016/S1872-2067(24)60081-1","DOIUrl":"10.1016/S1872-2067(24)60081-1","url":null,"abstract":"<div>Metal halide perovskite (MHP) has become one of the most promising materials for photocatalytic CO2 reduction owing to the wide light absorption range, negative conduction band position and high reduction ability. However, photoreduction of CO2 by MHP remains a challenge because of the slow charge separation and transfer. Herein, a cobalt single-atom modified nitrogen-doped graphene (Co-NG) cocatalyst is prepared for enhanced photocatalytic CO2 reduction of bismuth-based MHP Cs3Bi2Br9. The optimal Cs3Bi2Br9/Co-NG composite exhibits the CO production rate of 123.16 μmol g–1 h–1, which is 17.3 times higher than that of Cs3Bi2Br9. Moreover, the Cs3Bi2Br9/Co-NG composite photocatalyst exhibits nearly 100% CO selectivity as well as impressive long-term stability. Charge carrier dynamic characterizations such as Kelvin probe force microscopy (KPFM), single-particle PL microscope and transient absorption (TA) spectroscopy demonstrate the vital role of Co-NG cocatalyst in accelerating the transfer and separation of photogenerated charges and improving photocatalytic performance. The reaction mechanism has been demonstrated by in situ diffuse reflectance infrared Fourier-transform spectroscopy measurement. In addition, in situ X-ray photoelectron spectroscopy test and theoretical calculation reveal the reaction reactive sites and reaction energy barriers, demonstrating that the introduction of Co-NG promotes the formation of *COOH intermediate, providing sufficient evidence for the highly selective generation of CO. This work provides an effective single-atom-based cocatalyst modification strategy for photocatalytic CO2 reduction and is expected to shed light on other photocatalytic applications.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"64 ","pages":"Pages 143-151"},"PeriodicalIF":15.7,"publicationDate":"2024-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142122550","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}

引用次数: 0

S-scheme heterojunction with ultrafast interfacial electron transfer for artificial photosynthesis 用于人工光合作用的具有超快界面电子传递功能的 S 型异质结

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-09-01 DOI: 10.1016/S1872-2067(24)60102-6

Sihang Mao, Rongan He, Shaoqing Song

引用次数: 0

C–H bond activation of propane on Ga2O22+ in Ga/H-ZSM-5 and its mechanistic implications Ga/H-ZSM-5 中 Ga2O22+ 上丙烷的 C-H 键活化及其机理影响

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-09-01 DOI: 10.1016/S1872-2067(24)60065-3

Zhaoqi Zhao, Yunzhu Zhong, Xiaoxia Chang, Bingjun Xu

{"title":"C–H bond activation of propane on Ga2O22+ in Ga/H-ZSM-5 and its mechanistic implications","authors":"Zhaoqi Zhao, Yunzhu Zhong, Xiaoxia Chang, Bingjun Xu","doi":"10.1016/S1872-2067(24)60065-3","DOIUrl":"10.1016/S1872-2067(24)60065-3","url":null,"abstract":"<div>Propane dehydrogenation (PDH) on Ga/H-ZSM-5 catalysts is a promising reaction for propylene production, while the detail mechanism remains debatable. Ga2O22+ stabilized by framework Al pairs have been identified as the most active species in Ga/H-ZSM-5 for PDH in our recent work. Here we demonstrate a strong correlation between the PDH activity and a fraction of Ga2O22+ species corresponding to the infrared GaH band of higher wavenumber (GaHHW) in reduced Ga/H-ZSM-5, instead of the overall Ga2O22+ species, by employing five H-ZSM-5 supports sourced differently with comparable Si/Al ratio. This disparity in Ga2O22+ species stems from their differing capacity in completing the catalytic cycle. Spectroscopic results suggest that PDH proceeds via a two-step mechanism: (1) C–H bond activation of propane on H-Ga2O22+ species (rate determining step); (2) β-hydride elimination of adsorbed propyl group, which only occurs on active Ga2O22+ species corresponding to GaHHW.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"64 ","pages":"Pages 32-43"},"PeriodicalIF":15.7,"publicationDate":"2024-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142122655","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}

引用次数: 0