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学者姓名：龙金林
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Abstract ：
CH3OH is the most desired product of photocatalytic CH4 conversion. The prominent metal-decorated photocatalyst is challenging in both high yield and selectivity for CH3OH products due to over-oxidation by center dot OH mechanism. Here, interstitial Zn is fabricated into ZniO to induce the formation of Zn atom island for rapid single electron reduction of O2 into center dot OOH instead of center dot OH for the selective combination with methyl into CH3OOH. AuPd alloy is simultaneously decorated on ZniO surface for tuning CH3OOH adsorption and reduction into CH3OH. The synergy of Zn atom island and AuPd alloy achieve a tandem reaction pathway (CH4 -> CH3OOH -> CH3OH) for an unprecedented CH3OH yield of 2444 mmol gAuPd-1 h-1 (or 8800 mu mol gcat-1 h-1) with 98.3% selectivity, which bypasses the center dot OH mechanism for tuning the high selectivity of CH3OH. An apparent quantum efficiency of 18.53% at 370 nm for CH4 conversion are super to the reported photocatalytic systems. Thus, this work provides the new strategy of the synergetic atom island and metal alloy photocatalysts through a tandem reaction pathway to mediate the photocatalytic selective oxidation of CH4 into the desired CH3OH.
Keyword ：
atom island atom island AuPd alloy AuPd alloy methanol selectivity methanol selectivity photocatalysis photocatalysis tandem reaction tandem reaction
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| GB/T 7714 | Xiao, Zhen , Shen, Jinni , Jiang, Jianing et al. Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
| MLA | Xiao, Zhen et al. "Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH" . | ADVANCED FUNCTIONAL MATERIALS (2025) . |
| APA | Xiao, Zhen , Shen, Jinni , Jiang, Jianing , Zhang, Jiangjie , Liang, Shuqi , Han, Shitong et al. Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH . | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
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Aiming to improve the decay in thermochemical energy storage (TCES) performance of CaO-based looping materials with the number of carbonation/calcination cycles, a series of Y/Mg-codoped CaO-based materials were prepared by using the classical sol-gel method and citric acid as a carbon template to enhance the porosity and specific surface area. The structural characterizations showed that Y and Mg were presented in two forms. Part of Y/Mg was presented in the form of Y2O3 and MgO nanoparticles with an average size of 15 and 40 nm, respectively. These Y2O3 and MgO nanoparticles with high Tammann temperature and thermal conductivity were highly dispersed to retard the sintering and growth of CaO grains. The rest of Y and Mg were doped into the framework of the CaO lattice in atomic form by substituting Ca atoms. These Y and Mg created a large amount of the oxygen vacancies surrounding Ca atoms to facilitate the electron transfer from Ca2+ ions to dopants, which enhanced the CO2 capture capacity of CaO-based materials by improving the kinetics of the carbonation reaction. As a result, the optimal CaO-based composite denoted as Ca/Y5/Mg10 exhibited a high initial energy storage density of up to >2300 kJ/kg and held an excellent looping reaction stability after 25 carbonation/calcination cycles owing to the cooperation of Y with Mg additives. This work provided effective and economical CaO-based looping materials for application in thermochemical energy storage.
Keyword ：
CaO-based materials CaO-based materials carbonation/calcination cycles carbonation/calcination cycles sintering resistance sintering resistance thermochemical energy storage thermochemical energy storage Y/Mg codoping Y/Mg codoping
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| GB/T 7714 | Wang, Jifu , Xiong, Wei , Ding, Zhengxin et al. Enhancing the Stability of CaO-Based Looping Materials in Thermochemical Energy Storage by Codoping Y and Mg [J]. | ACS APPLIED ENERGY MATERIALS , 2024 , 7 (24) : 12165-12173 . |
| MLA | Wang, Jifu et al. "Enhancing the Stability of CaO-Based Looping Materials in Thermochemical Energy Storage by Codoping Y and Mg" . | ACS APPLIED ENERGY MATERIALS 7 . 24 (2024) : 12165-12173 . |
| APA | Wang, Jifu , Xiong, Wei , Ding, Zhengxin , Wang, Pengzhao , Long, Jinlin . Enhancing the Stability of CaO-Based Looping Materials in Thermochemical Energy Storage by Codoping Y and Mg . | ACS APPLIED ENERGY MATERIALS , 2024 , 7 (24) , 12165-12173 . |
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Halogenated methane serves as a universal platform molecule for building high-value chemicals. Utilizing sodium chloride solution for photocatalytic methane chlorination presents an environmentally friendly method for methane conversion. However, competing reactions in gas-solid-liquid systems leads to low efficiency and selectivity in photocatalytic methane chlorination. Here, an in situ method is employed to fabricate a hydrophobic layer of TaOx species on the surface of NaTaO3. Through in-situ XPS and XANES spectra analysis, it is determined that TaOx is a coordination unsaturated species. The TaOx species transforms the surface properties from the inherent hydrophilicity of NaTaO3 to the hydrophobicity of TaOx/NaTaO3, which enhances the accessibility of CH4 for adsorption and activation, and thus promotes the methane chlorination reaction within the gas-liquid-solid three-phase system. The optimized TaOx/NaTaO3 photocatalyst has a good durability for multiple cycles of methane chlorination reactions, yielding CH3Cl at a rate of 233 mu mol g(-1) h(-1) with a selectivity of 83%. In contrast, pure NaTaO3 exhibits almost no activity toward CH3Cl formation, instead catalyzing the over-oxidation of CH4 into CO2. Notably, the activity of the optimized TaOx/NaTaO3 photocatalyst surpasses that of reported noble metal photocatalysts. This research offers an effective strategy for enhancing the selectivity of photocatalytic methane chlorination using inorganic chlorine ions.
Keyword ：
hydrophobicity hydrophobicity methane chlorination methane chlorination photocatalysis photocatalysis TaOx TaOx ultrathin layer ultrathin layer
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| GB/T 7714 | Li, Dongmiao , Lin, Min , Zhang, Jiangjie et al. Hydrophobic TaOx Species Overlayer Tuning Light-Driven Methane Chlorination with Inorganic Chlorine [J]. | SMALL , 2024 , 20 (38) . |
| MLA | Li, Dongmiao et al. "Hydrophobic TaOx Species Overlayer Tuning Light-Driven Methane Chlorination with Inorganic Chlorine" . | SMALL 20 . 38 (2024) . |
| APA | Li, Dongmiao , Lin, Min , Zhang, Jiangjie , Qiu, Chengwei , Chen, Hui , Xiao, Zhen et al. Hydrophobic TaOx Species Overlayer Tuning Light-Driven Methane Chlorination with Inorganic Chlorine . | SMALL , 2024 , 20 (38) . |
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This work introduces a new strategy of a single-atom nest catalyst, whereby several single atoms are positioned closely, aiming to achieve the dual benefits of high atom-utilization efficiency while avoiding the steric hindrance in the coupling reaction. As a proof of concept, Pt single-atom nests, where the adjacent Pt single atoms are approximately 4 Å apart, are precisely engineered on the TiO2 photocatalyst for photocatalytic non-oxidative coupling of methane. The Pt single-atom nest photocatalyst demonstrates remarkable activity, achieving a C2H6 yield and turnover frequency of 251.6 μmol gcat-1 h-1 and 20 h-1, respectively, representing a 3.2-fold improvement compared to the Pt single-atom photocatalyst. Density functional theory calculations reveal that the Pt single-atom nest can significantly decrease the energy barrier for the activation of both CH4 molecules in the coupling process. © 2024 American Chemical Society.
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| GB/T 7714 | Zhang, P. , Li, J. , Huang, H. et al. Platinum Single-Atom Nests Boost Solar-Driven Photocatalytic Non-Oxidative Coupling of Methane to Ethane [J]. | Journal of the American Chemical Society , 2024 , 146 (34) : 24150-24157 . |
| MLA | Zhang, P. et al. "Platinum Single-Atom Nests Boost Solar-Driven Photocatalytic Non-Oxidative Coupling of Methane to Ethane" . | Journal of the American Chemical Society 146 . 34 (2024) : 24150-24157 . |
| APA | Zhang, P. , Li, J. , Huang, H. , Sui, X. , Zeng, H. , Lu, H. et al. Platinum Single-Atom Nests Boost Solar-Driven Photocatalytic Non-Oxidative Coupling of Methane to Ethane . | Journal of the American Chemical Society , 2024 , 146 (34) , 24150-24157 . |
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光催化水分解制氢是解决环境污染和能源危机的理想途径.共价有机骨架(COFs)作为一类由共价键连接的周期性网状拓扑材料,其电子结构和化学性质可在分子水平上进行定制和调控,是研究半导体光催化剂构-效关系的理想模型.为了提高COFs的电荷分离效率,在COFs骨架上设计供体-受体(D-A)单元,构筑分子内电场(IMEF)促进电荷定向迁移是一种行之有效的策略.然而,在亚胺键连接的COFs中,亚胺键取向诱导产生的键内电场(IBEF)对光生激子的分离效率的影响往往被忽视.因此,进一步研究IMEF与IBEF之间的相互作用对COFs内光生电子转移动力学的影响具有重要意义,可为深入揭示光催化产氢机制提供关键信息. 本文报道了一种基于COFs的双电场叠加策略,用于提高光催化产氢反应效率.首先,通过将有机单元的末端官能团进行互换,利用水热法成功制备了两种亚胺键取向相反的强D-A型COFs光催化剂,TNCA和TCNA.其中,官能团的微小变化保证了由D-A结构组成的IMEF方向和强度的一致性,可以使得在仅改变IBEF的情况下全面研究COFs的电子结构.X射线粉末衍射、傅里叶变换红外光谱、固体核磁以及X射线光电子能谱等结果证实了两种COFs的成功合成.随后,扫描电镜、透射电镜和氮气等温吸脱附曲线结果表明两种COFs均为介孔材料.紫外-可见漫反射光谱结果表明,所制备的催化剂具有良好的可见光吸收能力,结合莫特肖特基曲线结果,表明催化剂在热力学上均满足光催化产氢的要求.采用光致发光光谱、时间分辨荧光光谱、电子顺磁共振、光电流以及电化学阻抗研究了两种催化剂的载流子分离和转移行为,并且利用飞秒瞬态吸收光谱进一步明确了COFs中光生电荷转移动力学过程.结果表明,相较于TCNA,TNCA在光照下能够产生更多的光生电子且具有更长的寿命.光催化产氢活性评价结果显示,在可见光(A ≥ 420nm)照射下,具有同向叠加电场的TNCA,光催化析氢速率高达57.3 mmol·g-1·h-1,是具有相反电场取向TCNA(0.11 mmol·g-1·h-1)的520倍.并且TNCA具有更负的导带能级,有利于光生电子参与还原过程,最终获得较好的光催化析氢性能.此外,理论计算结果表明,当IMEF和IBEF取向一致时,亚胺键不仅可以为载流子迁移提供强大的驱动力,而且还能够有效地抑制载流子复合,进一步提高光生电子的利用率. 综上所述,本文提出了双电场叠加增强光生载流子高效分离的有效策略,为设计具有特定电场性质的COFs光催化材料提供了理论及实际参考.
Keyword ：
光催化 光催化 共价有机框架 共价有机框架 分子内电场 分子内电场 制氢 制氢 键内电场 键内电场
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| GB/T 7714 | 厉超 , 王朔 , 刘媛 et al. 共价有机框架双电场叠加实现高效光催化产氢 [J]. | 催化学报 , 2024 , 63 (8) : 164-175 . |
| MLA | 厉超 et al. "共价有机框架双电场叠加实现高效光催化产氢" . | 催化学报 63 . 8 (2024) : 164-175 . |
| APA | 厉超 , 王朔 , 刘媛 , 黄细河 , 庄严 , 吴舒鸿 et al. 共价有机框架双电场叠加实现高效光催化产氢 . | 催化学报 , 2024 , 63 (8) , 164-175 . |
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Efficient photocatalytic reduction of CO2 to high-calorific-value CH4, an ideal target product, is a blueprint for C-1 industry relevance and carbon neutrality, but it also faces great challenges. Herein, we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst, which are prepared via a facile impregnation-reduction method, featuring an optimized local electronic structure. It exhibits a superior photocatalytic carbon-based products yield of 30.0 mu mol g(-1) h(-1) and achieves a record CH4 selectivity of up to 94.3%, which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and selectivity. Specifically, the synergistic effects of directional migration of photogenerated electrons and strong pi-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO2 -> CH4 pathway. This study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.
Keyword ：
artificial synthesis of CH4 artificial synthesis of CH4 electronic structure optimization electronic structure optimization Fe species cocatalyst Fe species cocatalyst photocatalytic CO2 reduction photocatalytic CO2 reduction SiC SiC
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| GB/T 7714 | Lin, Qianying , Zhao, Jiwu , Zhang, Pu et al. Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation [J]. | CARBON ENERGY , 2024 , 6 (1) . |
| MLA | Lin, Qianying et al. "Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation" . | CARBON ENERGY 6 . 1 (2024) . |
| APA | Lin, Qianying , Zhao, Jiwu , Zhang, Pu , Wang, Shuo , Wang, Ying , Zhang, Zizhong et al. Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation . | CARBON ENERGY , 2024 , 6 (1) . |
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Photothermal catalytic N-acetylation of aniline has been a promising strategy to synthesize amides, which combined the advantages of thermal catalysis and photocatalysis. Herein, we demonstrate a high-performance strategy to synthesize amides catalyzed by the in-situ formed first-row transition-metal (Fe, Co, Ni, Mn et al.) complexes nanodots (TMC NDs) under solar light excitation without using noble metals or strong acids. The dualfunctional nitriles substrates acted as the ligands to coordinate with transition-metal salts affording photosensitive TMC NDs with high solar-to-thermal energy conversion efficiency. Intramolecular charge transitions reduced the energy barrier of nitriles activation by weakening C---N bond and triggered near-field temperature rise via the electron-phonon scattering non-radiative pathway. The reaction system exhibited good tolerance to different functional groups, affording a series of amide derivatives. Such a dynamic coordination reaction mode and the in-situ formed TMC NDs opens new avenues toward solar-heat conversion via photon-phonon coupling in the field of chemical synthesis.
Keyword ：
Amide synthesis Amide synthesis N-acyl sources N-acyl sources Photon -phonon coupling Photon -phonon coupling Photothermal catalysis Photothermal catalysis Transition-metal complexes nanodots Transition-metal complexes nanodots
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| GB/T 7714 | Ma, Xiong-Feng , Xiao, Rui , Wei, Yingcong et al. Photothermal catalytic conversion of water and inert nitriles to amide activated by in-situ formed transition-metal-complex nanodots [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 344 . |
| MLA | Ma, Xiong-Feng et al. "Photothermal catalytic conversion of water and inert nitriles to amide activated by in-situ formed transition-metal-complex nanodots" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 344 (2024) . |
| APA | Ma, Xiong-Feng , Xiao, Rui , Wei, Yingcong , Zhang, Shaohui , Hu, Xiaoyi , Zhang, Ling et al. Photothermal catalytic conversion of water and inert nitriles to amide activated by in-situ formed transition-metal-complex nanodots . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 344 . |
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Photocatalytic oxidative coupling of methane (POCM) is a direct way for the methane transformation into >= C2 alkanes. However, the typical oxygen activation path often leads to the formation of strong oxidizing superoxide radical (O-2(-)) species, which makes the whole reaction face serious selectivity problems. Herein, we constructed N and oxygen vacancy dual active sites on TiO2{001} nanosheets (TiO2-NVo) to regulate the oxygen activation pathway and achieve a high activity and selectivity of photocatalytic OCM. Compared with ordinary Au/TiO2{001} nanosheets, the alkane yields of Au/TiO2-NVo are increased from 16 mu mol h(-1) to 32 mu mol h(-1), and the selectivity of alkanes increased from 61% to 93%. The performance is superior when compared with the reported till date in photocatalytic OCM in batch reactors. The superior performance originates from the unique N-V-o dual active sites for synergistically cleaving the detrimental O-2(-) into desirable mono-oxygen active species (O-) to suppress undesired overoxidation reaction. The formed O- species from O-2(-) dissociation, in turn, is active for the selective H abstraction of CH4 into center dot CH3 to improve the subsequent C-C coupling reaction on the Au nanocluster surface. This work provides a new approach of O-2 dissociation to address the overoxidation of methane in an aerobic environment for achieving highly selective CH4 conversion.
Keyword ：
dual sites dual sites high selectivity high selectivity O-2 dissociation O-2 dissociation oxidative coupling of methane oxidative coupling of methane photocatalysis photocatalysis
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| GB/T 7714 | Zhang, Jiangjie , Zhang, Junhui , Shen, Jinni et al. Regulation of Oxygen Activation Pathways to Optimize Photocatalytic Methane Oxidative Coupling Selectivity [J]. | ACS CATALYSIS , 2024 , 14 (6) : 3855-3866 . |
| MLA | Zhang, Jiangjie et al. "Regulation of Oxygen Activation Pathways to Optimize Photocatalytic Methane Oxidative Coupling Selectivity" . | ACS CATALYSIS 14 . 6 (2024) : 3855-3866 . |
| APA | Zhang, Jiangjie , Zhang, Junhui , Shen, Jinni , Li, Dongmiao , Long, Jinlin , Dai, Wenxin et al. Regulation of Oxygen Activation Pathways to Optimize Photocatalytic Methane Oxidative Coupling Selectivity . | ACS CATALYSIS , 2024 , 14 (6) , 3855-3866 . |
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Converting CO2 into hydrocarbons using solar energy enables the seamless integration of efficient solar energy utilization and carbon neutrality, presenting an efficacious solution to simultaneously tackle energy and environmental issues. However, challenges arise in controlling the selectivity of reduction products hinder its industrial application due to uncertainties in decisive factors. Given the complexity of the photocatalytic process, it is imperative to improve the understanding of the thermodynamic aspects (including consideration of both redox potential of photocatalysts and light absorption properties, activation of stable CO2 molecules, similarity in reduction potential of products) as well as kinetic obstacles (such as high adsorption potential, significant time disparity between charge separation and transfer, competition from side reactions). This Review offers a comprehensive analysis of the factors that govern product selectivity and explores effective strategies for enhancing catalytic performance based on recent advancements in photocatalytic CO2 reduction to diverse chemical compounds. These profound insights provide invaluable guidance for addressing challenges in practical applications of photocatalytic CO2 conversion.
Keyword ：
Activity Activity CO2 reduction CO2 reduction Photocatalysis Photocatalysis Reactionmechanism Reactionmechanism Selectivity Selectivity
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| GB/T 7714 | Wang, Shuowen , Wang, Jiashun , Wang, Ying et al. Insight into the Selectivity-Determining Step of Various Photocatalytic CO2 Reduction Products by Inorganic Semiconductors [J]. | ACS CATALYSIS , 2024 , 14 (14) : 10760-10788 . |
| MLA | Wang, Shuowen et al. "Insight into the Selectivity-Determining Step of Various Photocatalytic CO2 Reduction Products by Inorganic Semiconductors" . | ACS CATALYSIS 14 . 14 (2024) : 10760-10788 . |
| APA | Wang, Shuowen , Wang, Jiashun , Wang, Ying , Sui, Xiaoyu , Wu, Shuhong , Dai, Wenxin et al. Insight into the Selectivity-Determining Step of Various Photocatalytic CO2 Reduction Products by Inorganic Semiconductors . | ACS CATALYSIS , 2024 , 14 (14) , 10760-10788 . |
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Metal nanoparticle (NP) cocatalysts are widely investigated for their ability to enhance the performance of photocatalytic materials; however, their practical application is often limited by the inherent instability under light irradiation. This challenge has catalyzed interest in exploring high-entropy alloys (HEAs), which, with their increased entropy and lower Gibbs free energy, provide superior stability. In this study, 3.5 nm-sized noble-metal-free NPs composed of a FeCoNiCuMn HEA are successfully synthesized. With theoretic calculation and experiments, the electronic structure of HEA in augmenting the catalytic CO2 reduction has been uncovered, including the individual roles of each element and the collective synergistic effects. Then, their photocatalytic CO2 reduction capabilities are investigated when immobilized on TiO2. HEA NPs significantly enhance the CO2 photoreduction, achieving a 23-fold increase over pristine TiO2, with CO and CH4 production rates of 235.2 and 19.9 mu mol g(-1) h(-1), respectively. Meanwhile, HEA NPs show excellent stability under simulated solar irradiation, as well high-energy X-ray irradiation. This research emphasizes the promising role of HEA NPs, composed of earth-abundant elements, in revolutionizing the field of photocatalysis.
Keyword ：
high-entropy alloy high-entropy alloy nanoparticle nanoparticle noble-metal-free noble-metal-free photocatalytic CO2 reduction photocatalytic CO2 reduction
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| GB/T 7714 | Huang, Haowei , Zhao, Jiwu , Guo, Hele et al. Noble-Metal-Free High-Entropy Alloy Nanoparticles for Efficient Solar-Driven Photocatalytic CO2 Reduction [J]. | ADVANCED MATERIALS , 2024 , 36 (26) . |
| MLA | Huang, Haowei et al. "Noble-Metal-Free High-Entropy Alloy Nanoparticles for Efficient Solar-Driven Photocatalytic CO2 Reduction" . | ADVANCED MATERIALS 36 . 26 (2024) . |
| APA | Huang, Haowei , Zhao, Jiwu , Guo, Hele , Weng, Bo , Zhang, Hongwen , Saha, Rafikul Ali et al. Noble-Metal-Free High-Entropy Alloy Nanoparticles for Efficient Solar-Driven Photocatalytic CO2 Reduction . | ADVANCED MATERIALS , 2024 , 36 (26) . |
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