Rui Li , Pengfei Feng , Bonan Li , Jiayu Zhu , Yali Zhang , Ze Zhang , Jiangwei Zhang , Yong Ding
{"title":"Photocatalytic reduction of CO2 over porous ultrathin NiO nanosheets with oxygen vacancies","authors":"Rui Li , Pengfei Feng , Bonan Li , Jiayu Zhu , Yali Zhang , Ze Zhang , Jiangwei Zhang , Yong Ding","doi":"10.1016/S1872-2067(25)64687-0","DOIUrl":"10.1016/S1872-2067(25)64687-0","url":null,"abstract":"<div><div>In recent years, photocatalytic CO<sub>2</sub> reduction reaction has been recognized as a crucial approach to solve the greenhouse effect. However, the low concentration of CO<sub>2</sub> in the atmosphere necessitates a catalyst with excellent CO<sub>2</sub> enrichment capability. Herein, we designed and synthesized a series of NiO nanosheets featuring oxygen vacancies. Under the condition of pure CO<sub>2</sub> and photosensitizer [Ru(bpy)<sub>3</sub>]Cl<sub>2</sub>, the yield of CO reaches 16.8 μmol/h with a selectivity of 96%. Through characterization and theoretical calculations, we demonstrate that the presence of oxygen vacancies not only enhances the adsorption capacity of catalysts but also induces lattice distortion in NiO, leading to an increased dipole moment and formation of an internal electric field that facilitates photogenerated carrier separation. Furthermore, we conducted CO<sub>2</sub> reduction reactions under atmospheric condition and surprisingly observed a changing of selectivity from CO to CO and CH<sub>4</sub>. A series of control experiments showed that [Ru(bpy)<sub>3</sub>]Cl<sub>2</sub> acts as a reduction reaction site due to the presence of O<sub>2</sub> in the atmosphere. Simultaneously, oxygen promotes water splitting, which results in abundant proton generation and subsequent changes in carbon products.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"73 ","pages":"Pages 242-251"},"PeriodicalIF":15.7,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144572848","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}
Lifang Liu , Yejun Xiao , Xiangyang Guo , Shengye Jin , Fuxiang Zhang
{"title":"Facets-controllable synthesis of metal-organic frameworks via one supersaturation strategy to insight intrinsic facets effect","authors":"Lifang Liu , Yejun Xiao , Xiangyang Guo , Shengye Jin , Fuxiang Zhang","doi":"10.1016/S1872-2067(25)64719-X","DOIUrl":"10.1016/S1872-2067(25)64719-X","url":null,"abstract":"<div><div>The facets effect on the catalytic properties of inorganic compounds and metal-organic frameworks (MOFs) has been widely demonstrated, but the intrinsic facets effect free of interference of capping agents has not been discussed. Here we give a proof-of-concept illustration on the intrinsic facets effect by employing the popularly investigated NH<sub>2</sub>-MIL-125(Ti) MOFs with {001}, {111} and {100} facets controllably exposed as model photocatalysts, which were synthesized via a simple supersaturation strategy free of any capping agents. Compared to conventional synthetic routes with capping agents employed, the NH<sub>2</sub>-MIL-125(Ti) MOFs obtained in this work exhibit remarkably different physical and chemical properties such as surface wettability, charge separation as well as trend of facets effect on photocatalytic water splitting performance. The main reason has been unraveled to originate from unavoidable residue/influence of capping agents during the conventional facets-controlled synthetic routes leading to changed local surface structural environment as well as distinct charge separation property. Our results demonstrate the importance and feasibility of facets-controllable synthesis free of capping agents in getting insight into the intrinsic facets effect of MOFs-related materials.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"73 ","pages":"Pages 153-158"},"PeriodicalIF":15.7,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144572874","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}
Xiaochun Hu , Longgang Tao , Kun Lei , Zhiqiang Sun , Mingwu Tan
{"title":"Unraveling TiO2 phase effects on Pt single-atom catalysts for efficient CO2 conversion","authors":"Xiaochun Hu , Longgang Tao , Kun Lei , Zhiqiang Sun , Mingwu Tan","doi":"10.1016/S1872-2067(25)64699-7","DOIUrl":"10.1016/S1872-2067(25)64699-7","url":null,"abstract":"<div><div>Single-atom catalysts (SACs) offer a promising approach for maximizing noble metals utilization in catalytic processes. However, their performance in CO<sub>2</sub> hydrogenation is often constrained by the nature of metal-support interactions. In this study, we synthesized TiO<sub>2</sub> supported Pt SACs (Pt<sub>1</sub>/TiO<sub>2</sub>), with Pt single atoms dispersed on rutile (Pt<sub>1</sub>/R) and anatase (Pt<sub>1</sub>/A) phases of TiO<sub>2</sub> for the reverse water-gas shift (RWGS) reaction. While both catalysts maintained 100% CO selectivity over time, Pt<sub>1</sub>/A achieved a CO<sub>2</sub> conversion of 7.5%, significantly outperforming Pt<sub>1</sub>/R (3.6%). <em>In situ</em> diffuse reflectance infrared Fourier-transform spectroscopy and X-ray photoelectron spectroscopy revealed distinct reaction pathways: the COOH pathway was dominant on Pt<sub>1</sub>/A, whereas the –OH + HCO pathway was more competitive on Pt<sub>1</sub>/R. Analysis of electron metal-support interactions and energy barrier calculations indicated that Pt<sub>1</sub>/A better stabilized metallic Pt species and facilitates more favorable reaction pathways with lower energy barriers. These findings provide valuable insights for the design of more efficient SAC systems in CO<sub>2</sub> hydrogenation processes.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"73 ","pages":"Pages 186-195"},"PeriodicalIF":15.7,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144572877","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":"Boosting interfacial charge-transfer kinetics via core-shell MOF heterostructures with shared metal nodes","authors":"Weilai Yu","doi":"10.1016/S1872-2067(25)60706-1","DOIUrl":"10.1016/S1872-2067(25)60706-1","url":null,"abstract":"","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"73 ","pages":"Pages 8-11"},"PeriodicalIF":15.7,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144572964","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":"Recent advances and challenges in electrochemical CO2 reduction to CH4","authors":"Lei Xiong , Xianbiao Fu","doi":"10.1016/S1872-2067(25)64672-9","DOIUrl":"10.1016/S1872-2067(25)64672-9","url":null,"abstract":"<div><div>The electrochemical CO<sub>2</sub> reduction (ECR) to hydrocarbon products is an attractive pathway to decrease CO<sub>2</sub> emission and advance a carbon-neutral process. Among the products of ECR, methane (CH<sub>4</sub>) stands out due to its high calorific value, serving as the main component of natural gas. However, the development of ECR catalysts capable of producing CH<sub>4</sub> with both high activity and stability remains critically urgent. This review summarizes and explores the research progress and future application strategies for ECR toward CH<sub>4</sub> production. Combining experiments, <em>in-situ</em> characterizations, and theoretical calculations, this review examines mechanism of CH<sub>4</sub> formation in ECR. It then clarifies key factors affecting Cu-based catalysts for CH<sub>4</sub> production, including facet dependence, size effects, and valence states. Next, this review details emerging strategies such as sub-nanoscale catalysts, Cu/oxides interface engineering, and Cu surface modification. Finally, future directions highlight <em>in-situ</em> characterization, reactor design, and high-throughput screening, guiding industrial CH<sub>4</sub> production.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"73 ","pages":"Pages 39-61"},"PeriodicalIF":15.7,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144572939","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}
Qian Bai , Juanjuan Qi , Rongzhe Zhang , Zhiyuan Chen , Zihao Wei , Zhiyi Sun , Ziwei Deng , Xudong Yang , Qiangwei Li , Wenxing Chen , Lidong Wang
{"title":"High-spin configuration of asymmetric CoN1C2 coordination for boosting d-p orbital hybridization in Fenton-like reactions","authors":"Qian Bai , Juanjuan Qi , Rongzhe Zhang , Zhiyuan Chen , Zihao Wei , Zhiyi Sun , Ziwei Deng , Xudong Yang , Qiangwei Li , Wenxing Chen , Lidong Wang","doi":"10.1016/S1872-2067(25)64674-2","DOIUrl":"10.1016/S1872-2067(25)64674-2","url":null,"abstract":"<div><div>Asymmetric single-atom catalysts (ASACs) have attracted much attention owing to their excellent catalytic properties. However, the relationship between asymmetric coordination and the spin states of metal sites remains unclear. Additionally, the modulation of reactive oxygen species in Fenton-like reactions remains challenging. Herein, a novel strategy is reported for the rational design of highly loaded Co ASACs (CoN<sub>1</sub>C<sub>2</sub>/C<sub>2</sub>N) immobilized on three-dimensional flower-like C<sub>2</sub>N using an in situ-generated carbon defect method. In particular, the asymmetrically tricoordinated CoN<sub>1</sub>C<sub>2</sub>/C<sub>2</sub>N exhibited excellent catalytic activity for sulfachloropyridazine degradation, with a turnover frequency of 36.8 min<sup>–1</sup>. Experimental results and theoretical calculations revealed that the electron spin state of the Co-active sites was transferred from the low-spin configuration (<em>t</em><sub>2g</sub><sup>6</sup><em>e</em><sub>g</sub><sup>1</sup>) to the high-spin configuration (<em>t</em><sub>2g</sub><sup>5</sup><em>e</em><sub>g</sub><sup>2</sup>) owing to asymmetric coordination. The high-spin Co 3<em>d</em> orbital in CoN<sub>1</sub>C<sub>2</sub>/C<sub>2</sub>N possessed more unpaired electrons and therefore, had a strong ability to gain electrons from the O 2<em>p</em> orbitals of HSO<sub>5</sub><sup>–</sup>, boosting <em>d-p</em> orbital hybridization. More importantly, the spin-electron filling in the σ* orbital of high-spin Co 3<em>d</em>−O 2<em>p</em> accelerated the desorption of *SO<sub>5</sub><sup>•−</sup>, which acted as a rate-limiting step in the reaction, thus facilitating more <sup>1</sup>O<sub>2</sub> generation. This study provides an innovative synthetic route for practical ASACs and clarifies the critical relationship between structure and spin state, paving the way for advancements in environmental remediation and energy conversion applications.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"73 ","pages":"Pages 334-346"},"PeriodicalIF":15.7,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144572934","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}
Chang Shu , Xiaoju Yang , Peixuan Xie, Xuan Yang, Bien Tan, Xiaoyan Wang
{"title":"Long-term photocatalytic hydrogen peroxide production by hydroquinone-buffered covalent organic frameworks","authors":"Chang Shu , Xiaoju Yang , Peixuan Xie, Xuan Yang, Bien Tan, Xiaoyan Wang","doi":"10.1016/S1872-2067(25)64676-6","DOIUrl":"10.1016/S1872-2067(25)64676-6","url":null,"abstract":"<div><div>Photocatalytic hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production offers a sustainable route to convert water and oxygen into H<sub>2</sub>O<sub>2</sub> using solar energy. However, achieving long-term stability in photocatalysts remains a critical challenge due to mismatched kinetics between oxygen reduction (ORR) and water oxidation (WOR), which leads to hole accumulation and oxidative degradation. Here, we report a redox-mediated strategy to address this bottleneck by designing a hydroquinone-embedded covalent organic framework (Tz-QH-COF) that enables reversible hole buffering and kinetic balance. The hydroquinone (QH) units act as dynamic hole reservoirs, capturing excess holes during ORR and converting to benzoquinone (Q), which is regenerated to QH via WOR, thereby preventing oxidative decomposition. This reversible QH/Q cycle, directly visualized through <em>in situ</em> attenuated total reflection surface-enhanced infrared absorption spectroscopy, ensures unmatched stability, achieving continuous H<sub>2</sub>O<sub>2</sub> production for 528 h (22 d) with an accumulated yield of 18.6 mmol L<sup>–1</sup>—the highest reported duration for organic photocatalysts. Density functional theory calculations reveal that the QH units exhibit a strong oxygen adsorption energy and favorable two-electron ORR/WOR pathways with low energy barriers. The synergy between experimental and theoretical insights elucidates a redox-mediated charge-balance mechanism, advancing the design of robust photocatalysts for solar-driven H<sub>2</sub>O<sub>2</sub> synthesis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"73 ","pages":"Pages 300-310"},"PeriodicalIF":15.7,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144572945","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}
Haneul Shim , Sumin Pyo , Avnish Kumar , Yasin Khani , Siyoung Q. Choi , Kanghee Cho , Jechan Lee , Young-Kwon Park
{"title":"Improvement in the production of aromatics from pyrolysis of plastic waste over Ga-modified ZSM-5 catalyst under C1-gas environment","authors":"Haneul Shim , Sumin Pyo , Avnish Kumar , Yasin Khani , Siyoung Q. Choi , Kanghee Cho , Jechan Lee , Young-Kwon Park","doi":"10.1016/S1872-2067(25)64683-3","DOIUrl":"10.1016/S1872-2067(25)64683-3","url":null,"abstract":"<div><div>This study explores, for the first time, the influence of various C1 gases, such as methane (CH<sub>4</sub>), carbon dioxide (CO<sub>2</sub>), and biogas (CH<sub>4</sub> + CO<sub>2</sub>), on catalytic pyrolysis of plastic waste (polypropylene) to evaluate their potential in producing aromatic hydrocarbons. Also, this study used the 0.5 wt%, 1 wt%, 3 wt%, and 5 wt% Ga-modified ZSM-5 catalyst and its reduction-oxidation processed catalysts owing to their promising catalytic properties. According to the results, the highest yield (39.5 wt%) of BTEX (benzene, toluene, xylene, and ethylbenzene) was achieved under CH<sub>4</sub> over RO-GHZ(1) catalyst among all tested conditions. The reduction-oxidation process not only promotes a significant reduction of the Ga-size but also induces its diffusion inside the pore, compared to GHZ(1). This leads to the formation of highly active GaO<sup>+</sup> ionic species, balancing the Lewis/Brönsted ratio, thereby accelerating the aromatization reaction. The effect of Ga loading on the RO-GHZ catalyst was also evaluated systematically, which showed a negative impact on the BTEX yield owing to the lowering in the concentration of active GaO<sup>+</sup> species. A detailed catalyst characterization supports the experimental results well.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"73 ","pages":"Pages 368-383"},"PeriodicalIF":15.7,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144572936","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":"Recent advances in the preparation of glycolic acid by selective electrocatalytic oxidation of ethylene glycol","authors":"Jie Chen, Jing Li, Zidong Wei","doi":"10.1016/S1872-2067(25)64710-3","DOIUrl":"10.1016/S1872-2067(25)64710-3","url":null,"abstract":"<div><div>Ethylene glycol (EG) is a biomass derivative of polyethylene terephthalate (PET), and its electrocatalytic conversion into high-value chemicals has sparked widespread interest. This study reviews the most recent research development in electrocatalysis-based EG to glycolic acid (GA) conversion. Firstly, the strategies and research results of modulating the electronic structure of catalysts for efficient selective GA production from EG are reviewed. Second, by reviewing the data of <em>in-situ</em> Fourier transform infrared spectroscopy and <em>in-situ</em> electrochemically attenuated total reflection surface enhanced infrared absorption spectroscopy, the reaction pathway and catalytic mechanism of EG partial oxidation to GA were clarified. Finally, the design and regulation of catalysts for selective oxidation of EG by electrocatalysis in the future are prospected.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"73 ","pages":"Pages 79-98"},"PeriodicalIF":15.7,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144572941","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}
Chenhao Li , Hao Wang , Weiwei Wang , Shuo Bai , Zhongbin Gong , Qinqin Sang , Yuqing Zhang , Feng Huo , Yanrong Liu
{"title":"PtCu nano-dendrites with enhanced stability in proton exchange membrane fuel cells","authors":"Chenhao Li , Hao Wang , Weiwei Wang , Shuo Bai , Zhongbin Gong , Qinqin Sang , Yuqing Zhang , Feng Huo , Yanrong Liu","doi":"10.1016/S1872-2067(25)64712-7","DOIUrl":"10.1016/S1872-2067(25)64712-7","url":null,"abstract":"<div><div>The rigorous operating condition of proton exchange membrane fuel cells (PEMFCs) poses a substantial hurdle for the long-term stability of Pt-based alloy catalysts; thus, the development of Pt-alloy catalysts with unique morphologies is crucial for enhancing the stability of PEMFCs. In this study, we synthesized a novel PtCu nano-dendrite (PtCuND) catalyst through a facile, one-step solvothermal process. The sub-nanometer particles and nanopores within this catalyst facilitate enhanced mass transport. In PEM single-cell tests, the PtCuND catalyst displays high activity and robust stability, achieving a mass activity of 0.65 A mg<sub>Pt</sub><sup>–1</sup>. Notably, after accelerated durability tests, the mass activity and the voltage at 0.8 A cm<sup>–2</sup> of PtCuND exhibits only minimal decreases of 18.5% and 9 mV, respectively. The combined experimental results and theoretical calculations conclusively illustrate the optimized adsorption of oxygen species and the impact of compressive strain on the catalyst surface. The enhanced durability can be attributed to the maintained nano-dendritic morphology and the strengthened interaction within the Pt-Cu bonds. This work not only enhances the stability of PEMFCs but also provides a robust foundation for the future scaling up of catalyst production, paving the way for widespread application in sustainable energy systems.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"73 ","pages":"Pages 322-333"},"PeriodicalIF":15.7,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144572947","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}