Chinese Journal of Catalysis最新文献

{"title":"A superlattice interface and S-scheme heterojunction of Mn0.5Cd0.5S/MnWO4 for enhancing photocatalytic H2 production","authors":"Yanfeng Zhang , Shan Wang","doi":"10.1016/S1872-2067(24)60253-6","DOIUrl":"10.1016/S1872-2067(24)60253-6","url":null,"abstract":"","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 1-4"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143859520","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":"Tuning d-band electronic structure of Ni-Fe oxyhydroxides via doping engineering boosts seawater oxidation performance","authors":"Liyuan Xiao,&nbsp;Xue Bai,&nbsp;Jingyi Han,&nbsp;Zhenlu Wang,&nbsp;Jingqi Guan","doi":"10.1016/S1872-2067(24)60255-X","DOIUrl":"10.1016/S1872-2067(24)60255-X","url":null,"abstract":"<div><div>Seawater electrolysis holds significant importance for advancing clean energy conversion. NiFe-based catalysts exhibit outstanding performance in the oxygen evolution reaction (OER) under alkaline conditions. However, the instability of the Fe active center leads to leakage issues, hindering further development in the field of seawater electrolysis. Here, we adopt an element doping engineering strategy to enhance the OER activity of Ni-Fe oxyhydroxides and greatly stabilize the Fe sites by meticulously optimizing the <em>d</em>-band centers. Among the selected metals (Al, Ce, Co, Cr, Cu, Mn, Sn, Zn and Zr), Mn doping is the most effective as confirmed by both theoretical calculations and experimental verifications. The NiFeMn-OOH/NF formed <em>in situ</em> from the corresponding metal-organic framework requires only 217 mV to achieve a current density of 10 mA·cm^–2 in alkaline seawater, and exhibits exceptional stability. Theoretical calculations uncover that the Fe sites exhibit better balance of adsorption-desorption kinetics for OER intermediates than Ni sites and Ni-Fe dual-sites, while Mn sites with the polyvalent nature modulate the <em>d</em>-band center closer to Fermi level, facilitate the transfer of electrons across the catalyst surface, thus accelerating the reaction kinetics. This work is of considerable significance for achieving efficient and sustainable seawater electrolysis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 340-352"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860204","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":"Promoting stability of sub-3 nm In2S3 nanoparticles via sulfur anchoring for CO2 electroreduction to formate","authors":"Fanrong Chen ,&nbsp;Jiaju Fu ,&nbsp;Liang Ding ,&nbsp;Xiaoying Lu ,&nbsp;Zhe Jiang ,&nbsp;Xiaoling Zhang ,&nbsp;Jin-Song Hu","doi":"10.1016/S1872-2067(24)60233-0","DOIUrl":"10.1016/S1872-2067(24)60233-0","url":null,"abstract":"<div><div>The <em>p</em>-block metal (In, Sn, Bi, etc.)-based electrocatalysts have exhibited excellent activity in the electrocatalytic CO₂ reduction (ECR) to formate. However, the rapid decrease in catalytic activity caused by catalyst reconstruction and agglomeration under ECR conditions significantly restricts their practical applications. Herein, we developed a sulfur anchoring strategy to stabilize the high-density sub-3 nm In₂S₃ nanoparticles on sulfur-doped porous carbon substrates (i-In₂S₃/S-C) for formate production. Systematic characterizations evidenced that the as-prepared catalyst exhibited a strong metal sulfide-support interaction (MSSI), which effectively regulated the electronic states of In₂S₃, achieving a high formate Faradaic efficiency of 91% at −0.95 V <em>vs</em>. RHE. More importantly, the sulfur anchoring effectively immobilized the sub-3 nm In₂S₃ nanoparticles to prevent them from agglomeration. It enabled the catalysts to exhibit much higher durability than the In₂S₃ samples without sulfur anchoring, demonstrating that the strong MSSI and fast charge transfer on the catalytic interface could significantly promote the structural stability of In₂S₃ catalysts. These results provide a viable approach for developing efficient and stable electrocatalysts for CO₂ reduction.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 138-145"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860098","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":"CO2-promoted ethylbenzene dehydrogenation catalyzed by zeolite-encaged single chromium sites","authors":"Jian Dang ,&nbsp;Xin Deng ,&nbsp;Weijie Li ,&nbsp;Di Yang ,&nbsp;Guangjun Wu ,&nbsp;Landong Li","doi":"10.1016/S1872-2067(24)60241-X","DOIUrl":"10.1016/S1872-2067(24)60241-X","url":null,"abstract":"<div><div>The selective activation of C-H bonds is pivotal in catalysis for converting hydrocarbons into value-added chemicals. Ethylbenzene dehydrogenation to styrene is crucial process to produce polystyrene and its derivatives used in synthetic materials. Herein, K-Cr@Y with zeolite-encaged isolated O=Cr(VI)=O species modified by extraframework potassium ions is constructed, showing remarkable performance in CO₂-promoted ethylbenzene dehydrogenation with initial ethylbenzene conversion of 66% and styrene selectivity of 96%, outperforming other <em>M</em>-Cr@Y catalysts (<em>M</em> = Li, Na, Rb, Cs). Extraframework potassium ions can modulate the electron density of zeolite-encaged Cr(VI) species and therefore facilitate C–H bond activation in ethylbenzene molecules. The gradual reduction of zeolite-encaged O=Cr(VI)=O to less active Cr(IV)=O species by dihydrogen during ethylbenzene dehydrogenation is evidenced by comprehensive characterization results, and Cr(IV)=O can be re-oxidized to O=Cr(VI)=O species upon simple calcination regeneration. The results from <em>in situ</em> DRIFT spectroscopy elucidate the critical promotion role of CO₂ in ethylbenzene dehydrogenation over K-Cr@Y by retarding the over-reduction of zeolite-encaged Cr species to inactive Cr(III) species and suppressing coke deposition. This study advances the rational design of non-noble metal catalysts for CO₂-promoted ethylbenzene dehydrogenation with zeolite-encaged high valence transition metal ions modulated by extraframework cations.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 158-168"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143859528","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":"Highly efficient hydrogenation of NO to NH3 via a Fe2O3/TiO2 catalyst","authors":"Yanqin Li ,&nbsp;Wenlong Wang ,&nbsp;Junqi Tian ,&nbsp;Dan Cui ,&nbsp;Jun Yuan ,&nbsp;Bin Fang ,&nbsp;Nianliang Yin ,&nbsp;Zelong Li ,&nbsp;Feng Yu","doi":"10.1016/S1872-2067(24)60251-2","DOIUrl":"10.1016/S1872-2067(24)60251-2","url":null,"abstract":"<div><div>Nitrogen oxides (NO_<em>x</em>) present in flue gas are economically renewable N1 resources. Unlike traditional selective catalytic reduction processes that convert NO into N₂, redirecting NO towards the synthesis of value-added NH₃ offers significant practical benefits. In this study, a Ti-based metal-organic framework (Ti-MOF), specifically MIL-125, was utilized as a support for Fe, which was subsequently calcined at 400 °C to produce a Fe₂O₃/TiO₂-MOF catalyst. The resulting catalyst demonstrated exceptional performance, achieving 99% NO conversion and 95% NH₃ selectivity under optimal conditions of 450 °C, 0.1 MPa, and a gas hourly space velocity of 38000 mL g^–1 h⁻¹. Additionally, the catalyst exhibited excellent stability and resistance to water and sulfur. The high efficiency of Fe₂O₃/TiO₂-MOF is attributed to the abundance of Fe²⁺ sites at the reaction temperature, which enhances NO adsorption and activation. Furthermore, density functional theory calculations suggest that NO undergoes hydrogenation at the N-terminus on the Fe₂O₃/TiO₂-MOF surface, leading directly to NH₃ synthesis rather than dissociation followed by hydrogenation. This catalyst presents a novel approach for converting NO_<em>x</em> into high-value chemical products.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 330-339"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860203","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":"Improving enzymatic degradation of unpretreated poly(ethylene terephthalate)","authors":"Yufeng Cao ,&nbsp;La Xiang ,&nbsp;Jasmina Nikodinovic-Runic ,&nbsp;Veselin Maslak ,&nbsp;Jian-Ming Jin ,&nbsp;Chaoning Liang ,&nbsp;Shuang-Yan Tang","doi":"10.1016/S1872-2067(24)60232-9","DOIUrl":"10.1016/S1872-2067(24)60232-9","url":null,"abstract":"<div><div>Although the efficiency of poly(ethylene terephthalate) (PET) degradation has been successfully improved by depolymerase engineering, mostly by using Goodfellow-PET (gf-PET) as a substrate, efforts to degrade unpretreated PET materials with high crystallinity remain insufficient. Here, we endeavored to improve the degradation capability of a WCCG mutant of leaf-branch compost cutinase (LCC) on a unpretreated PET substrate (crystallinity &gt; 40%) by employing iterative saturation mutagenesis. Using this method, we developed a high-throughput screening strategy appropriate for unpretreated substrates. Through extensive screening of residues around the substrate-binding groove, two variants, WCCG-sup1 and WCCG-sup2, showed good depolymerization capabilities with both high- (42%) and low-crystallinity (9%) substrates. The WCCG-sup1 variant completely depolymerized a commercial unpretreated PET product in 36 h at 72 °C. In addition to enzyme thermostability and catalytic efficiency, the adsorption of enzymes onto substrates plays an important role in PET degradation. This study provides valuable insights into the structure-function relationship of LCC.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 375-389"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860207","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":"Strong interaction between Fe and Ti compositions for effective CO2 hydrogenation to light olefins","authors":"Hao Liang ,&nbsp;Shunan Zhang ,&nbsp;Ruonan Zhang ,&nbsp;Haozhi Zhou ,&nbsp;Lin Xia ,&nbsp;Yuhan Sun ,&nbsp;Hui Wang","doi":"10.1016/S1872-2067(24)60268-8","DOIUrl":"10.1016/S1872-2067(24)60268-8","url":null,"abstract":"<div><div>Fe-based catalysts are widely used for CO₂ hydrogenation to light olefins (C_2–4⁼); however, precise regulation of active phases and the balance between intermediate reactions remain significant challenges. Herein, we find that the addition of moderate amounts of Ti forms a strong interaction with Fe compositions, modulating the Fe₃O₄ and Fe₅C₂ contents. Enhanced interaction leads to an increased Fe₅C₂/Fe₃O₄ ratio, which in turn enhances the adsorption of reactants and intermediates, promoting CO hydrogenation to unsaturated alkyl groups and facilitating C–C coupling. Furthermore, the strong Fe-Ti interaction induces the preferential growth of Fe₅C₂ into prismatic structures that expose the (020), (–112), and (311) facets, forming compact active interfacial sites with Fe₃O₄ nanoparticles. These facet and interfacial effects significantly promote the synergistic coupling of the reverse water gas shift and Fischer-Tropsch reactions. The optimized 3K/FeTi catalyst with the highest Fe₅C₂/Fe₃O₄ ratio of 3.6 achieves a 52.2% CO₂ conversion rate, with 44.5% selectivity for C_2–4⁼ and 9.5% for CO, and the highest space-time yield of 412.0 mg g_cat^–1 h^–1 for C_2–4⁼.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 146-157"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143859527","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":"Peptide bridging for cofactor channeling in fusion enzyme lowers cofactor input by two orders of magnitude","authors":"Zehui Guo,&nbsp;Yan Sun","doi":"10.1016/S1872-2067(24)60231-7","DOIUrl":"10.1016/S1872-2067(24)60231-7","url":null,"abstract":"<div><div>Biocatalysis with nicotinamide adenine dinucleotide phosphate (NADP)-dependent oxidoreductases faces a challenge in improving the efficiency of the costly cofactor utilization. Although enzyme fusion can offer cofactor regeneration, the high-volume input and limited cofactor recyclability still make the enzymatic processes unsustainable. Therefore, it is of great significance to reduce cofactor input in a fusion enzyme (FuE) system, but no successful practice has been reported. Herein, we design a decapeptide bridge, RRRQRRRARR (R10), with high affinity for NADPH to construct fusion oxidoreductases (phenylacetone monooxygenase and phosphite dehydrogenase) for ester synthesis and NADP recycling. The peptide bridge enables electrostatic cofactor channeling that transports NADPH/NADP⁺ across the peptide between the enzymes’ NADP-binding pockets, so the fusion enzyme (FuE-R10) presents 2.1-folds and 2.0-folds higher conversions than mixed free enzymes and a flexible linker (GGGGSGGGGS)-fused enzyme, respectively, at NADPH/FuE of 0.1. The fusion enzyme, FuE-R5, bridged by a half-shortened linker, is proved more effective in facilitating cofactor channeling; compared to the mixed free enzymes, FuE-R5 exhibits two orders of magnitude reduction of NADPH input in ester synthesis. The work has thus demonstrated the potential of the cofactor bridging strategy in the development of sustainable cofactor-dependent cascade biocatalysis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 390-403"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860094","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":"Chemistry of CeO2-derived nanocomposites photocatalysts for environment monitoring and energy conversion","authors":"Anees A. Ansari ,&nbsp;Ruichan Lv ,&nbsp;Shili Gai ,&nbsp;Piaoping Yang","doi":"10.1016/S1872-2067(24)60266-4","DOIUrl":"10.1016/S1872-2067(24)60266-4","url":null,"abstract":"<div><div>Photocatalysis is an important process in energy conversion and environmental usage because of its feasible, profitable, and environmentally safe benefits. Coordination chemistry of the CeO₂ is gaining significant interest because its nanocomposites show unique characteristics namely optically active, wide bandgap (<em>E</em>_g), reversible valence states (Ce^3+/4+), rich defect architectures, high O₂ storage capability, ionic conductivity, and exceptional chemical resistance. Systematically summarized the importance of synthesis methods, particle morphology, and crystal structure aiming at how to heighten the efficacy of CeO₂-derived hybrid heterojunction (HHJ) photocatalyst. Selection of an appropriate synthesis method and morphology of the composite materials are beneficial in inhibiting the rapid electron-hole (<em>e</em>⁻-<em>h</em>⁺) recombination, improvement in visible light adsorption, and large generation of <em>e</em>⁻-<em>h</em>⁺ pairs to accelerate the photocatalysts activities. Various modification approaches include elemental doping (metal/non-metal doping), heterojunction construction (lower/wide <em>E</em>_g semiconductors (SCD), carbon, conducting polymeric materials), imperfection engineering, and multicomponent hybrid composites. These methods assist as a valuable resource for the rational design of effective CeO₂-based composite photocatalysts for sustainable development owing to the enhancement of oxygen species mobility, rapid charge transfer, maximum visible light captivation and slow down the charge recombination rate with increase photogeneration of <em>e</em>⁻-<em>h</em>⁺ pairs. Also examines the advancements made in CeO₂ conjugated hybrid composites in photo-oxidation of wastewater effluents (antibiotic/organic dyes/chemical/pharmaceutical), heavy metal removal, H₂ production, CO₂ reduction, and H₂O splitting applications. Subsequently, the difficulties and fundamental ideas behind several heterojunction photocatalysts encountered by CeO₂-based composites are examined, and future directions for their development are suggested.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 70-113"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143859526","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":"Accelerating C-C coupling in alkaline electrochemical CO2 reduction by optimized local water dissociation kinetics","authors":"Qingfeng Hua ,&nbsp;Hao Mei ,&nbsp;Guang Feng ,&nbsp;Lina Su ,&nbsp;Yanan Yang ,&nbsp;Qichang Li ,&nbsp;Shaobo Li ,&nbsp;Xiaoxia Chang ,&nbsp;Zhiqi Huang","doi":"10.1016/S1872-2067(24)60243-3","DOIUrl":"10.1016/S1872-2067(24)60243-3","url":null,"abstract":"<div><div>Electrochemical carbon dioxide reduction reaction (CO₂RR) produces valuable chemicals by consuming gaseous CO₂ as well as protons from the electrolyte. Protons, produced by water dissociation in alkaline electrolyte, are critical for the reaction kinetics which involves multiple proton coupled electron transfer steps. Herein, we demonstrate that the two key steps (CO₂-*COOH and *CO-*COH) efficiency can be precisely tuned by introducing proper amount of water dissociation center, <em>i.e.</em>, Fe single atoms, locally surrounding the Cu catalysts. In alkaline electrolyte, the Faradaic efficiency (FE) of multi-carbon (C₂₊) products exhibited a volcano type plot depending on the density of water dissociation center. A maximum FE for C₂₊ products of 73.2% could be reached on Cu nanoparticles supported on N-doped Carbon nanofibers with moderate Fe single atom sites, at a current density of 300 mA cm^–2. Experimental and theoretical calculation results reveal that the Fe sites facilitate water dissociation kinetics, and the locally generated protons contribute significantly to the CO₂ activation and *CO protonation process. On the one hand, <em>in-situ</em> attenuated total reflection surface-enhanced infrared absorption spectroscopy (<em>in-situ</em> ATR-SEIRAS) clearly shows that the *COOH intermediate can be observed at a lower potential. This phenomenon fully demonstrates that the optimized local water dissociation kinetics has a unique advantage in guiding the hydrogenation reaction pathway of CO₂ molecules and can effectively reduce the reaction energy barrier. On the other hand, abundant *CO and *COH intermediates create favorable conditions for the asymmetric *CO-*COH coupling, significantly increasing the selectivity of the reaction for C₂₊ products and providing strong support for the efficient conversion of related reactions to the target products. This work provides a promising strategy for the design of a dual sites catalyst to achieve high FE of C₂₊ products through the optimized local water dissociation kinetics.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"71 ","pages":"Pages 128-137"},"PeriodicalIF":15.7,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860097","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}