Chinese Journal of Catalysis最新文献

Dual-hole extraction strategy promotes photoelectrochemical water splitting of bismuth vanadate photoanode 双孔萃取策略促进了钒酸铋光阳极的电化学水分解

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64778-4

Hua Yang , Dingyanyan Zhou , Kaige Tian , Lingjiang Kong , Pengfei An , Jing Zhang , Yujin Ji , Youyong Li , Junqing Yan

{"title":"Dual-hole extraction strategy promotes photoelectrochemical water splitting of bismuth vanadate photoanode","authors":"Hua Yang , Dingyanyan Zhou , Kaige Tian , Lingjiang Kong , Pengfei An , Jing Zhang , Yujin Ji , Youyong Li , Junqing Yan","doi":"10.1016/S1872-2067(25)64778-4","DOIUrl":"10.1016/S1872-2067(25)64778-4","url":null,"abstract":"<div><div>Elemental doping of BiVO4 crystal lattices effectively enhances carrier separation, thereby facilitating efficient photoelectrochemical water splitting. However, the positive effect of elementally induced lattice distortions on hole extraction has been neglected. Herein, the crystal lattice of BiVO4 is distorted by doping with an inexpensive Cs metal; then, CoFe2O4 is used as an efficient hole-extraction layer to further modify the surface of the doped photoanode. Benefiting from the above design, the newly prepared CoFe2O4-Cs-BiVO4 photoanode achieved a photocurrent density of 5.66 mA cm–2 at 1.23 V vs. a reversible hydrogen electrode, indicating a 3.9-fold improvement in photocurrent density. Detailed physicochemical characterization and density functional theory calculations showed that the lattice distortion induced by Cs doping promoted the directional migration of BiVO4 bulk-phase holes to the CoFe2O4 layer. Additionally, the coupled CoFe2O4 can be used as a hole extraction layer to further enhance the interfacial migration of carriers. The synergistic effect of the two effectively promotes the directional migration of photogenerated carriers from the BiVO4 bulk phase to the active sites of the oxygen evolution reaction, thereby effectively inhibiting carrier recombination. This study revealed the positive effect of the dual-hole extraction strategy on solar energy conversion, thereby opening new avenues for the rational design of photoanodes.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 236-249"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145061246","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

Synergistic interface engineering in Cu-Zn-Ce catalysts for efficient CO2 hydrogenation to methanol Cu-Zn-Ce催化剂催化CO2加氢制甲醇的协同界面工程

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64773-5

Yang Chen , Diwen Zhou , Yongli Chang , Hongqiao Lin , Yunzhao Xu , Yong Zhang , Ding Yuan , Lizhi Wu , Yu Tang , Chengyi Dai , Xingang Li , Qinhong Wei , Li Tan

{"title":"Synergistic interface engineering in Cu-Zn-Ce catalysts for efficient CO2 hydrogenation to methanol","authors":"Yang Chen , Diwen Zhou , Yongli Chang , Hongqiao Lin , Yunzhao Xu , Yong Zhang , Ding Yuan , Lizhi Wu , Yu Tang , Chengyi Dai , Xingang Li , Qinhong Wei , Li Tan","doi":"10.1016/S1872-2067(25)64773-5","DOIUrl":"10.1016/S1872-2067(25)64773-5","url":null,"abstract":"<div><div>CO2 hydrogenation to CH3OH is of great significance for achieving carbon neutrality. Here, we show a urea-assisted grinding strategy for synthesizing Cu-Zn-Ce ternary catalysts (CZC-G) with optimized interfacial synergy, achieving superior performance in CO2 hydrogenation to methanol. The CZC-G catalyst demonstrated exceptional methanol selectivity (96.8%) and a space-time yield of 73.6 gMeOH·kgcat–1·h–1 under optimized conditions. Long-term stability tests confirmed no obvious deactivation over 100 h of continuous operation. Structural and mechanistic analyses revealed that the urea-assisted grinding method promotes the formation of Cu/Zn-Ov-Ce ternary interfaces and inhibits the reduction of ZnO, enabling synergistic interactions for efficient CO2 activation and selective stabilization of formate intermediates (HCOO*), which are critical for methanol synthesis. In-situ diffuse reflectance infrared Fourier transform spectra and X-ray absorption spectroscopy studies elucidated the reaction pathway dominated by the formate mechanism, while suppressing the reverse water-gas shift reaction. This work underscores the critical role of synthetic methodologies in engineering interfacial structures, offering a strategy for designing high-performance catalysts for sustainable CO2 resource utilization.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 171-183"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145061311","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

In-situ SEIRAS for dynamic single-atom catalysis 动态单原子催化的原位SEIRAS

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64789-9

Haifeng Qi, Graham J. Hutchings

引用次数: 0

Constructing high-entropy spinel oxide thin films via magnetron sputtering for efficiently electrocatalyzing alkaline oxygen evolution reaction 磁控溅射制备高熵尖晶石氧化薄膜，用于高效电催化碱性析氧反应

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64771-1

Yuhui Chen, Congbao Guo, Yi Wang, Kun Wang, Shuqin Song

{"title":"Constructing high-entropy spinel oxide thin films via magnetron sputtering for efficiently electrocatalyzing alkaline oxygen evolution reaction","authors":"Yuhui Chen, Congbao Guo, Yi Wang, Kun Wang, Shuqin Song","doi":"10.1016/S1872-2067(25)64771-1","DOIUrl":"10.1016/S1872-2067(25)64771-1","url":null,"abstract":"<div><div>Ensuring high electrocatalytic performance simultaneously with low or even no precious-metal usage is still a big challenge for the development of electrocatalysts toward oxygen evolution reaction (OER) in anion exchange membrane water electrolysis. Here, homogeneous high entropy oxide (HEO) film is in-situ fabricated on nickel foam (NF) substrate via magnetron sputtering technology without annealing process in air, which is composed of many spinel-structured (FeCoNiCrMo)3O4 grains with an average particle size of 2.5 nm. The resulting HEO film (abbreviated as (FeCoNiCrMo)3O4) exhibits a superior OER performance with a low OER overpotential of 216 mV at 10 mA cm–2 and steadily operates at 100 mA cm–2 for 200 h with a decay of only 272 μV h–1, which is far better than that of commercial IrO2 catalyst (290 mV, 1090 μV h–1). Tetramethylammonium cation (TMA+) probe experiment, activation energy analysis and theoretical calculations unveil that the OER on (FeCoNiCrMo)3O4 follows an adsorbate evolution mechanism pathway, where the energy barrier of rate-determining step for OER on (FeCoNiCrMo)3O4 is substantially lowered. Also, methanol molecular probe experiment suggests that a weakened *OH bonding on the (FeCoNiCrMo)3O4 surface and a rapid deprotonation of *OH, further enhancing its OER performance. This work provides a feasible solution for designing efficient high entropy oxides electrocatalysts for OER, accelerating the practical process of water electrolysis for H2 production.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 210-219"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145061243","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

Mechanistic insights into sulfation-induced deactivation of CoMn2O4/CeTiOx catalyst under low-temperature SCR conditions 低温SCR条件下磺化诱导CoMn2O4/CeTiOx催化剂失活机理研究

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64781-4

Ning Luo , Fengyu Gao , Chengzhi Wang , Honghong Yi , Shunzheng Zhao , Yuansong Zhou , Shangfeng Du , Xiaolong Tang

{"title":"Mechanistic insights into sulfation-induced deactivation of CoMn2O4/CeTiOx catalyst under low-temperature SCR conditions","authors":"Ning Luo , Fengyu Gao , Chengzhi Wang , Honghong Yi , Shunzheng Zhao , Yuansong Zhou , Shangfeng Du , Xiaolong Tang","doi":"10.1016/S1872-2067(25)64781-4","DOIUrl":"10.1016/S1872-2067(25)64781-4","url":null,"abstract":"<div><div>The problem of water and sulfur poisoning in flue gas atmosphere remains a significant obstacle for low-temperature deNOx catalysts. This study investigated the sulfation mechanism of the CoMn2O4/CeTiOx (CMCT) catalyst during the selective catalytic reduction of NOx with NH3 under conditions containing H2O and SO2 at 150 °C. Employing a comprehensive suite of time-resolved analysis and characterization techniques, the evolution of sulfate species was systematically categorized into three stages: initial rapid surface sulfate accumulation, the transformation of surface sulfates to bulk metal sulfates, and partial sulfates decomposition after the removal of H2O and SO2. These findings indicate that bulk metal sulfates irreversibly deactivate the catalyst by distorting active component lattices and consuming oxygen vacancies, whereas surface sulfates (including ammonium sulfates and surface-coordinated metal sulfates) cause reversible performance loss through decomposition. Furthermore, the competitive adsorption of H2O and SO2 significantly influences the catalytic efficiency, with H2O suppressing SO2 adsorption while simultaneously enhancing the formation of Brönsted acid sites. This research underscores the critical role of sulfate dynamics on catalyst performance, revealing the enhanced SO2 resistance of the Eley-Rideal mechanism facilitated by the Ce-Ti support relative to the Langmuir-Hinshelwood pathway. Collectively, the study unravels the complex interplay of sulfate dynamics influencing catalyst performance and provides potential approaches to mitigate deactivation in demanding atmospheric conditions.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 70-86"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145060780","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

Quantitative correlation of Fe(III) electronic structure regulation in peroxymonosulfate activation via atomic cobalt doping AgFeO2 原子钴掺杂AgFeO2对过氧单硫酸盐活化中Fe（III）电子结构调控的定量关联

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64784-X

Chen Xu , Di Song , Xinggang Liu , Fang Deng , Yongcai Zhang , Mingshan Zhu , Xijun Liu , Jianping Zou , Xubiao Luo

{"title":"Quantitative correlation of Fe(III) electronic structure regulation in peroxymonosulfate activation via atomic cobalt doping AgFeO2","authors":"Chen Xu , Di Song , Xinggang Liu , Fang Deng , Yongcai Zhang , Mingshan Zhu , Xijun Liu , Jianping Zou , Xubiao Luo","doi":"10.1016/S1872-2067(25)64784-X","DOIUrl":"10.1016/S1872-2067(25)64784-X","url":null,"abstract":"<div><div>The influence of electronic structure on the performance of catalysts for peroxymonosulfate (PMS) activation remains ambiguous. In this study, the 3d electron configuration of Fe(III) in AgFeO2 was atomically regulated using cobalt doping. The amount of PMS adsorbed and the catalytic performance were positively correlated with the total effective magnetic moment and the ratios of high-spin Fe(III) and eg filling within the catalysts. These 3d electron regulations favor PMS adsorption and electron transfer owing to the lower PMS adsorption energy, increased electronic states near the Fermi level, and reduced dz2 orbital occupancy. Benefiting from fine tailoring of the electron configuration, the AgFe0.80Co0.20O2 catalyst exhibited outstanding catalytic PMS activation and favorable application potential, achieving efficient pharmaceutical wastewater treatment and more than 80% ofloxacin removal after 72 h of continuous-flow operation. Notably, this study offers a comprehensive understanding for the influence mechanism of electronic structure regulation on PMS activation, providing design guidance for the development of efficient heterogeneous Fenton-like catalytic systems.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 87-98"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145060781","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

Non-thermal plasma to boost lattice oxygen activation in Ce1-xCoxO2-δ catalysts for efficient soot combustion at low temperatures 非热等离子体提高Ce1-xCoxO2-δ催化剂的晶格氧活性，用于低温高效煤烟燃烧

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64775-9

Feiyang Zhang , Yanjun Chen , Mengyao Sun , Peng Wang , Yuxin Miao , Zhongyang Zheng , Shixin Liu , Xuehua Yu , Zhen Zhao

{"title":"Non-thermal plasma to boost lattice oxygen activation in Ce1-xCoxO2-δ catalysts for efficient soot combustion at low temperatures","authors":"Feiyang Zhang , Yanjun Chen , Mengyao Sun , Peng Wang , Yuxin Miao , Zhongyang Zheng , Shixin Liu , Xuehua Yu , Zhen Zhao","doi":"10.1016/S1872-2067(25)64775-9","DOIUrl":"10.1016/S1872-2067(25)64775-9","url":null,"abstract":"<div><div>Effective lattice oxygen (Olatt) activation at low temperatures has long been a challenge in catalytic oxidation reactions. Traditional thermal catalytic soot combustion, even with Pt/Pd catalysts, is inefficient at exhaust temperatures below 200 °C, particularly under conditions of frequent idling. Herein, we report an effective strategy utilizing non-thermal plasma (NTP) to activate Olatt in Ce1–xCoxO2–δ catalysts, achieving dramatic enhancement of the soot combustion rate at low temperatures. At 200 °C and 4.3 W (discharge power, Pdis), NTP-Ce0.8Co0.2O2–δ achieved 96.9% soot conversion (XC), 99.0% CO2 selectivity (S(CO2)) and a maximum energy conversion efficiency (Emax) of 14.7 g kWh–1. Compared with previously reported results, NTP-Ce0.8Co0.2O2–δ exhibits the highest S(CO2) and Emax values. Remarkably, even without heating, XC, Emax, and S(CO2) reached 92.1%, 6.1 g kWh–1, and 97.5%, respectively, at 6.3 W (Pdis). The results of characterization and theoretical calculation demonstrated that Co dopes into the CeO2 crystal lattice and forms an asymmetric Ce–O–Co structure, making oxygen “easy come, easy go”, thereby enabling the rapid combustion of soot over NTP-Ce0.8Co0.2O2–δ. This study highlights the great potential of NTP for activating Olatt and provides valuable insights into the design of efficient NTP-adapted catalysts for oxidation reactions.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 99-109"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145060776","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

Integrated design of iridium-based catalysts for proton exchange membrane water electrolyzers 质子交换膜水电解槽用铱基催化剂的集成设计

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64787-5

Jiahao Yang , Zhaoping Shi , Minhua Shao , Meiling Xiao , Changpeng Liu , Wei Xing

{"title":"Integrated design of iridium-based catalysts for proton exchange membrane water electrolyzers","authors":"Jiahao Yang , Zhaoping Shi , Minhua Shao , Meiling Xiao , Changpeng Liu , Wei Xing","doi":"10.1016/S1872-2067(25)64787-5","DOIUrl":"10.1016/S1872-2067(25)64787-5","url":null,"abstract":"<div><div>Proton exchange membrane water electrolysis (PEMWE) has garnered significant attention as a pivotal technology for converting surplus electricity into hydrogen for long-term storage, as well as for providing high-purity hydrogen for aerospace and high-end manufacturing applications. With the ongoing commercialization of PEMWE, advancing iridium-based oxygen evolution reaction (OER) catalysts remains imperative to reconcile stringent requirements for high activity, extended longevity, and minimized noble metal loading. The review provides a systematic analysis of the integrated design of iridium-based catalysts in PEMWE, starting from the fundamentals of OER, including the operation environment of OER catalysts, catalytic performance evaluation within PEMWE, as well as catalytic and dissolution mechanisms. Subsequently, the catalyst classification and preparation/characterization techniques are summarized with the focus on the dynamic structure-property relationship. Guided by these understandings, an overview of the design strategies for performance enhancement is presented. Specifically, we construct a mathematical framework for cost-performance optimization to offer quantitative guidance for catalyst design. Finally, future perspectives are proposed, aiming to establish a theoretical framework for rational catalyst design.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 20-44"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145060778","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

Origin of Brönsted acidity in germanosilicates from neighboring Ge-hydroxyl groups 锗硅酸盐中邻近ge -羟基Brönsted酸性的来源

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64762-0

Kun Lu , Qian Liu , Liyu Chen , Jilong Wang , Zhenxuan Yuan , Xiao Kong , Yunxing Bai , Jingang Jiang , Yejun Guan , Sicong Ma , Hao Xu , Weixin Huang , Zhipan Liu , Peng Wu

{"title":"Origin of Brönsted acidity in germanosilicates from neighboring Ge-hydroxyl groups","authors":"Kun Lu , Qian Liu , Liyu Chen , Jilong Wang , Zhenxuan Yuan , Xiao Kong , Yunxing Bai , Jingang Jiang , Yejun Guan , Sicong Ma , Hao Xu , Weixin Huang , Zhipan Liu , Peng Wu","doi":"10.1016/S1872-2067(25)64762-0","DOIUrl":"10.1016/S1872-2067(25)64762-0","url":null,"abstract":"<div><div>Constructing new Brönsted acid sites within zeolitic materials holds paramount importance for the advancement of solid-acid catalysis. Zeo-type germanosilicates, a class of metallosilicates with a neutral framework composed of tetravalent Ge and Si oxygen tetrahedrons, are conventionally considered not to generate Brönsted acid sites. Herein, we disclose an abnormal phenomenon with Ge-rich IWW-type germanosilicate (IWW-A) as an example that Ge-enriched germanosilicates are featured by mild Brönsted acidity. Using the art-of-state density functional theory calculation, 19F magic angle spinning nuclear magnetic resonance, microcalorimetric and ammonia infrared mass spectrometry- temperature-programmed desorption characterizations, the nature of germanosilicate’s Brönsted acidity has been demonstrated to be closely related to the neighboring framework Ge-hydroxyl pairs. Besides, the contribution of Ge-OH groups to Brönsted acidity and the role of Ge-pair structure for maintaining mild acid strength have been elucidated. In catalytic cracking of n-hexane and methanol-to-olefins reaction, the IWW-A germanosilicate exhibit high light olefins selectivity, good recyclability and low carbon deposition, outperforming the benchmark zeolite catalyst, ZSM-5 aluminosilicate.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 110-122"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145060782","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

Remote hydrogen-spillover effect on catalytic transnitrilation for biomass-based nitrile synthesis 远距离氢溢出效应对生物质基腈合成催化透硝化的影响

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64782-6

Guipeng Zhang, Yan Bin, Yanxin Wang, Jinzhu Chen

{"title":"Remote hydrogen-spillover effect on catalytic transnitrilation for biomass-based nitrile synthesis","authors":"Guipeng Zhang, Yan Bin, Yanxin Wang, Jinzhu Chen","doi":"10.1016/S1872-2067(25)64782-6","DOIUrl":"10.1016/S1872-2067(25)64782-6","url":null,"abstract":"<div><div>Acid-nitrile exchange reaction (transnitrilation) is a state-of-the-art strategy for nitrile synthesis with a promising industrial application. Herein, a dedicated catalytic system for transnitrilation was designed based on remote H-spillover effect by physically mixing Pt nanoparticles-encapsulated in hollow ZSM-5 (Pt@ZSM-5) and Ni-doped Nb2O5 (Ni/Nb2O5) under 10%-H2/N2. The Pt@ZSM-5 acts as a primary active-center for H2-dissociation over Pt to form H-spillover; while, Ni/Nb2O5 serves as an acceptor-site of H-spillover. Upon uptake of the H-spillover, the doped-reversible Ni2+/Ni+ couples in the Ni/Nb2O5 significantly facilitate migrations of proton (Brönsted-acid site) and surface vacancy (Lewis-acid site) throughout its surface, thus enhancing and enriching its surface-acidic sites for the catalytic transnitrilation. Kinetic analysis demonstrates nitrile-activation over Lewis-acid site of Ni/Nb2O5 as rate-determining step of the transnitrilation. This research provides a molecular-scale and fundamental understanding of remote H-spillover effect on a solid acid for an improved catalytic performance by in-situ regulation on its surface-acid type and strength.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 153-170"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145060730","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