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Unveiling the promotion role of ZnO on Zn-Al spinel oxide for CO2 hydrogenation

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Journal of Energy Chemistry 2025年第1期100卷 18-25页

作者： Tongyao Wang Xinlong Yao Lixin Liang Hongyu Chen Pan Gao Guangjin Hou State Key laboratory of Catalysis Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences

The Zn-Al spinel oxide stands out as one of the most active catalysts for high-temperature methanol synthesis from CO2hydrogenation. However, the structure–activity relationship of the reaction remains poorly understood due to challenges in atomic-level structural characterizations and analysis of reaction intermediates. In this study, we prepared two Zn-Al spinel oxide catalysts via coprecipitation（ZnAl-C）and hydrothermal（ZnAl-H） methods, and conducted a comparative investigation in the CO2hydrogenation reaction. Surprisingly, under similar conditions, ZnAl-C exhibited significantly higher selectivity towards methanol and DME compared to ZnAl-H. Comprehensive characterizations using X-ray diffraction（XRD）, Raman spectroscopy and electron paramagnetic resonance（EPR） unveiled that ZnAl-C catalyst had abundant ZnO species on its surface, and the interaction between the ZnO species and its ZnAl spinel oxide matrix led to the formation of oxygen vacancies, which are crucial for CO2adsorption and activation. Additionally, state-of-the-art solid-state nuclear magnetic resonance（NMR） techniques,including ex-situ and in-situ NMR analyses, confirmed that the surface ZnO facilitates the formation of unique highly reactive interfacial formate species, which was readily hydrogenated to methanol and DME. These insights elucidate the promotion effects of ZnO on the ZnAl spinel oxide in regulating active sites and reactive intermediates for CO2-to-methanol hydrogenation reaction, which is further evidenced by the significant enhancement in methanol and DME selectivity observed upon loading ZnO onto the ZnAl-H catalyst. These molecular-level mechanism understandings reinforce the idea of optimizing the ZnO-ZnAl interface through tailored synthesis methods to achieve activity-selectivity balance.

关键词： Reaction intermediates

Experimental Study on Diesel Spray and Flame Asymmetry Characteristics of Dual-Orifice Nozzles for a Medium-Speed Engine

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Journal of Thermal Science 2025年第1期34卷 303-322页

作者： JU Dehao LIU Rui ZHENG Liang DENG Jiahui ZHANG Wenzheng HUO Jinlu HUANG Li Shanghai Marine Diesel Engine Research Institute National Key laboratory of Marine Engine Science and Technology Key laboratory for Power Machinery and Engineering Ministry of EducationShanghai Jiao Tong University

The asymmetry of the multi-orifice spray will cause uneven heat load of the marine diesel engine,thereby affecting its working performance and service ***,an in-depth understanding of the spray and flame characteristics of multi-orifice nozzles will guide the optimization of the nozzle structure,needle design and diesel atomization and combustion *** this reason,four groups of dual-orifice nozzles with different hole diameters(0.1-0.55 mm) and mass flow rates covering the typical marine medium-speed diesel injections are designed and customized,and the constant volume chamber(CVC) with high temperature and pressure is used to simulate the actual in-cylinder working conditions of the diesel engine for the spray visualization *** study the asymmetry of the fuel sprays discharged from a diesel injector,the multi-orifice nozzle is simplified as a dual-orifice nozzle in this *** with X-ray Computed Tomography(CT) imaging technology,the influences of the nozzle internal structure on the spray and flame asymmetry are studied in the constructed supercritical *** is found that the asymmetry of the inlet angle and the equivalent length-diameter ratio is positively correlated with the inconsistency of the dual *** an increase in the injection pressure and nozzle diameter,the asymmetry of the dual spray becomes more pronounced,resulting in greater disparities in the ignition delay times and ignition positions of the two ***,the increase in nozzle diameter also leads to combustion instability,resulting in a flame with a serrated *** the increase of ambient temperature,the proportion of liquid phase in the jet decreases and the relative density of spray front decreases.

关键词： atomization dual-orifice nozzle nozzle structure spray flame asymmetry

Plasmonic tandem heterojunctions enable high-efficiency charge transfer for broad spectrum photocatalytic hydrogen production

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Journal of Energy Chemistry 2025年第1期100卷 710-720页

作者： Wenxuan Chen Xiu-Qing Qiao Guo Hui Bojing Sun Dongfang Hou Meidi Wang Xueqian Wu Tao Wu Dong-Sheng Li College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials China Three Gorges University Hubei Three Gorges laboratory College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Supramolecular Coordination Chemistry Jinan University

Rational engineering of semiconductor photocatalysts for efficient hydrogen production is of great significance but still challenging,primarily due to the limitations in charge transfer ***,a fascinating plasmonic tandem heterojunction with the hc-CdS/Mo2C@C heterostructure is aimfully prepared for effectively promoting the charge separation kinetics of the CdS photocatalyst via the synergistic strategy of phase junction,Schottky junction,and photothermal *** difference in atomic configuration between cubic-CdS （c-CdS） and hexagonal-CdS （h-CdS） leads to effective charge separation through a typical Ⅱ charge transfer mechanism,and plasmonic Schottky junction further extracts the electrons in the hc-CdS phase junction to realize gradient charge ***,the photothermal effect of Mo2C@C helps to expand the light absorption,accelerate charge transfer kinetics,and reduce the hydrogen evolution energy *** carbon layer provides a fast channel for charge transfer and protects the photocatalyst from *** a result,the optimized hc-CMC photocatalyst exhibits a significantly high photocatalytic H2production activity of 28.63 mmol/g/h and apparent quantum efficiency of 61.8%,surpassing most of the reported *** study provides a feasible strategy to enhance the charge transfer kinetics and photocatalytic activity of CdS by constructing plasmonic tandem heterogeneous junctions.

关键词： Cadmium sulfide

Gradient maturation experiment on hairs implies taphonomic changes in fossil hairs

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Science China Earth Sciences 2025年第1期68卷 62-73页

作者： Xin LI Yibo ZHOU Tao ZHAO Xingjian HE Yanhong PAN State Key laboratory for Mineral Deposits Research Center for Critical Earth Material Cycling Centre for Research and Education on Biological Evolution and Environment and Frontiers Science School of Earth Sciences and Engineering Nanjing University Institute of Palaeontology Yunnan Key Laboratory of Earth System Science Yunnan Key Laboratory for PalaeobiologyYunnan University

Mammalian hair, as a key feature related to endothermy, physical protection, and camouflage, has a long geohistorical record that dates back even to the Mesozoic. However, the limited information on the taphonomy of hair hinders the understanding of its evolutionary significance in deep time. To address this, we conducted taphonomic experiments to simulate the transformation process of black hair. The changes in the morphological structure, microscopic characteristics, and chemical composition of hair during the simulated fossilization process were documented by scanning electron microscopy, Fourier transform infrared(FTIR) spectroscopy, and Raman spectroscopy. Our results revealed that damage to the morphology of hair began at a mild temperature(150–175°C), and hair transformed into a fluid-like mass at a relatively high temperature(200°C). In addition, the morphological structure of melanosomes had relatively greater preservation potential than keratins did, and the microscopic features of melanosomes were persistently stable. The Raman and FTIR spectra indicated that the characteristic melanin and keratin peaks changed as the temperature increased. Although the chemical signals were not lost completely, the variations in the characteristic amide bands in the FTIR spectra indicate that the keratins severely degraded at high temperatures(>200°C), whereas the characteristic melanin bands in the Raman spectra suggested that melanin signals were still recognizable, even at high temperatures(>200°C). These results were confirmed by principal component analysis(PCA) and principal component analysis linear discriminant analysis(PCA–LDA). In addition, the Raman signals of all the samples in the simulated experiments were distinguished from the signals of common geological carbonaceous materials(humic acid), which suggested that Raman spectroscopy can be used to detect melanin in fossils.

关键词： Mammalian hair Melanin Keratin Fossilization Experimental taphonomy

Oxygen vacancies enriched Ir/WOx catalysts for the directly chem-catalytic conversion of cellulose to ethanol

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Tungsten 2025年第1期7卷 88-99页

作者： Yu-Jing Weng Zhao-Ying Ding Ying-Chao Li Yuan-Feng Wu Yuan-Yang Xu Rui Chen Xiao-Lei Zhao Hai-Yong Wang Da-Lei Zhang Yu-Long Zhang Henan Key laboratory of Coal Green Conversion and International Joint Laboratory of Coal Clean Utilization College of Chemistry and Chemical Engineering Henan Polytechnic University Key laboratory of Renewable Energy Guangzhou Institute of Energy Conversion Chinese Academy of Sciences Liaoning Institute of Energy Technology

Tungsten and its oxides are highly versatile catalysts with unique properties that hold great promise for a wide array of applications,including biological pathways and chemical *** chemo-catalysis of cellulose to ethanol presents a promising avenue for ethanol synthesis with the potential for enhanced efficiency compared to conventional methods,offering a sustainable and carbon-neutral alternative to existing petrochemical and biological ***,Ir/WOxcatalysts enriched with oxygen vacancies were meticulously prepared and demonstrated remarkable catalytic performance in converting cellulose to ethanol directly in the presence of tungstic *** catalyst achieved a high ethanol yield of 66.5%under optimal reaction conditions,approaching the theoretical yield limit of traditional ethanol *** results revealed the presence of oxygen defects,Bronsted/Lewis acidity,and Ir nanoclusters on the catalyst surface,working synergistically to facilitate the cascade catalysis of cellulose hydrolysis,sugar retro-aldol condensation reaction,and C2 intermediate hydrodeoxygenation to *** situ Fourier transform infrared spectrometer analysis confirmed the catalyst's ability to enhance the adsorption and activation of ethylene glycol for ethanol *** manipulating subtle structural features,this study offers a fresh perspective on tungsten group catalyst design and underscores the importance of synergistic effects among catalytic sites for the efficient production of ethanol from cellulose.

关键词： Cellulosic ethanol Chem-catalysis Hydrogenolysis Retro-aldol condensation Tungsten

Low-cost and fluoride-free synthesis of MFI zeolite nanosheets with enhanced stability for benzene alkylation with ethanol

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Journal of Energy Chemistry 2025年第1期100卷 458-468页

作者： Peng Zhu Cun Liu Yiren Yu Guoshu Gao Yumeng Zhao Xiongfu Zhang Guodong Liu Guohui Yang State Key laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology State Key laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented *** obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.

关键词： Aspect ratio

Crustal magma oxidation state and endowments in porphyry copper deposits

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Science China Earth Sciences 2025年第1期68卷 226-236页

作者： Yumin AI Massimo CHIARADIA Chao WU Huayong CHEN Key laboratory of Mineralogy and Metallogeny Guangzhou Institute of Geochemistry Chinese Academy of Sciences University of Chinese Academy of Sciences Department of Earth Sciences University of Geneva Guangdong Provincial Key laboratory of Mineral Physics and Materials

Porphyry copper deposits（PCDs） supply the majority of the world's copper（Cu） as well as significant amounts of molybdenum（Mo） and gold（Au）. The formation of these deposits is controlled by a variety of geological factors, among which the magmatic oxidation is one of the focuses of current research. This study investigates the redox characteristics of arc magmas by analyzing the ratio of vanadium（V） to scandium（Sc） and its correlation with the oxygen fugacity （fO2） of magmas from arcs of various crustal thicknesses globally. We compiled an extensive dataset of published V/Sc values and studied the partition coefficients of Vand Sc between minerals and silicate melts across various magmatic environments. The results demonstrate that fractional crystallization of magnetite markedly reduces V/Sc values of the residual melt. Furthermore, magnesium number（Mg#） at the onset of magnetite fractionation is strongly positively correlated with fO2of the equilibrium magma. Based on this,the oxidation of arc magmas from different crustal thicknesses can be evaluated. The result suggests that magmas generated in crusts thicker than 20 km tend to be more oxidized with increasing crust thickness. This trend is attributed to enhanced intracrustal differentiation processes involving garnet and amphibole, particularly in mature island and continental arcs. In contrast,magmas in thinner arc crusts（<20 km）, which are significantly influenced by subducted slab materials, display higher oxidation states than most of their thicker crust counterparts. These findings suggest that both subduction dynamics and crustal thickness play a vital role in determining the oxidation state of arc magmas and, consequently, their capacity to generate PCDs. Highly oxidized, primitive arc magmas are less favorable for PCD formation due to that they tend to experience magnetite fractionation and thus sulfide saturation in the early stage of magma evolution, a process leading to copper depletion. On the contra

关键词： Magma evolution V/Sc systematics Magnetite Oxygen fugacity Porphyry copper deposits

New insight into the origin and evolution of the flora and fauna of Hainan Island, China

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Science China Earth Sciences 2025年第1期68卷 52-61页

作者： Hua ZHU Center for Integrative Conservation Xishuangbanna Tropical Botanical Garden Chinese Academy of Sciences Yunnan International Joint Laboratory of Southeast Asia Biodiversity Conservation Yunnan Key Laboratory for the Conservation of Tropical Rainforests and Asian Elephants

The origin of the biota of Hainan Island, China, remains a fundamental scientific problem. Comparative studies on the biota, geological tectonics, and paleomagnetism proposed that during the Eocene, Hainan Island connected Vietnam and Guangxi, and then moved to the southeast to reach its present location. This review mainly discusses its biota origin from molecular phylogeny and palaeobotanical research. The formation and evolution of the biological groups of Hainan Island were identified via research on their genomes, phylogeny, and molecular biogeography. This research showed that the genera and species that appeared and diverged early in their evolution(i.e., before the Miocene) can be explained by the land connection between Hainan Island, Vietnam, and Guangxi during the Eocene-Oligocene. According to Southeast Asian tectonic theory, in the Middle Miocene(at about 15 million years ago), Hainan Island had moved to its present position. The population and genetic divergence of species with late divergence times(after 15 Ma) can be reasonably explained by the close proximity(or land connection) between Hainan Island and the Leizhou Peninsula, enabling genetic communication between Hainan Island and the Chinese mainland, but have exceptional cases. Conclusions have been obtained through palaeobotanical studies, showing that in the Eocene-Oligocene period, southwest China and Hainan Island had subtropical vegetation and flora. However, the fossil group in southeast China(in Maoming, near present-day Hainan Island) in the Late Eocene indicated a tropical rainforest vegetation and flora. This suggests that in the Paleogene, Hainan Island may have been located near or on the southwest border of Guangxi and northern Vietnam, rather than in its present location. The floristic division of the flora of Hainan Island basically presents a northeast-southwest inclined distribution pattern. This pattern can be explained by the counterclockwise rotation of Hainan Island during i

关键词： Molecular phylogeny Biogeography Paleobotany Origin of flora and fauna Hainan Island of China

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Recent progress on photoactive nonprecious transition-metal complexes

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Science China Chemistry 2025年第1期68卷 46-95页

作者： Zhong-Liang Gong Hong-Jie Zhang Yan Cheng Jianxun Liu Yuhan Ai Yaqin Li Zhihui Feng Qiong Zhang Shaolong Gong Yong Chen Chang-Jiang Yao Yuan-Yuan Zhu Liang-Jin Xu Yu-Wu Zhong CAS Key laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences State Key laboratory of Structural Cemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences School of Chemistry and Chemical Engineering Anhui Key Laboratory of Advanced Catalytic Materials and Reaction EngineeringHefei University of Technology State Key laboratory of Explosion Science and Safety Protection School of Mechatronical Engineering Beijing Institute of Technology College of Chemistry and Molecular Sciences Hubei Key Lab on Organic and Polymeric Optoelectronic Materials Wuhan University School of Chemistry and Chemical Engineering Anhui University Key laboratory of Photochemical Conversion and Optoelectronic Materials & CAS-HKU Joint laboratory on New Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences

Photoactive complexes of nonprecious transition metals, mainly including those in the first-row and partially the second-row of the Periodic table of elements, have received increasing attention in view of their low cost and long-term sustainability. They are recognized as promising alternatives to noble transition metal complex congeners that have been extensively studied in optoelectronic devices, artificial photosynthesis, photocatalysis, biodiagnostics, and therapeutics, etc. This review is devoted to a comprehensive summary on the classical and recent advances on photoactive nonprecious transition metal complexes, including photoactive Zr, V, Cr, Mo, and W complexes, Mn complexes and hybrids, Fe, Co, Ni, and Cu complexes, and Zn and Cd complexes and hybrids. A particular focus is given on the molecular design, modulation of photophysical and photochemical properties, and applications of the representative and lately-developed nonprecious metal complexes. In addition, a perspective on the future development in this field is provided at the end of this review.

关键词： photoactive metal complexes earth-abundant metals nonprecious metal complexes luminescence photochemistry