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学者姓名：张宏伟
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Abstract ：
The capture the low-content NH3 from industrial streams, and recycle it as the feedstocks for industrial processes is very important. In this work, we reported the use of mesoporous polydivinylbenzene (PDVB) as the support of metal-based deep eutectic solvents (DESs) containing choline chloride (ChCl) and metal chlorides (SnCl2, FeCl3 or ZnCl2) for NH3 capture. The structure of composite materials was characterized in details, and the NH3 capture performance and mechanism of them were also examined in depth. Owing to the coordination interaction of metal ions with NH3, along with the hydrogen-bond interaction of - OH and Cl- with NH3, the DES@PDVB composites exhibit considerably high low-content NH3 capacities. The optimized sample ChCl + 2ZnCl2@PDVB1.5 can adsorb 7.43 mol/kg of NH3 at 25 degree celsius and 0.122 bar, which is advantageous over most other adsorbents fabricated in the literature. The mechanism of NH3 capture by DES@PDVB composites was also illustrated through spectroscopic characterizations.
Keyword ：
Deep eutectic solvent Deep eutectic solvent Low content Low content Mesoporous polymer Mesoporous polymer Multiple interaction Multiple interaction NH 3 capture NH 3 capture
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| GB/T 7714 | Zhang, Jiayin , Fang, Siqi , Zheng, Lu et al. Mesoporous polymer supported Metal-Based deep eutectic solvents for enhanced capture of Low-Content Ammonia [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 493 . |
| MLA | Zhang, Jiayin et al. "Mesoporous polymer supported Metal-Based deep eutectic solvents for enhanced capture of Low-Content Ammonia" . | CHEMICAL ENGINEERING JOURNAL 493 (2024) . |
| APA | Zhang, Jiayin , Fang, Siqi , Zheng, Lu , Cao, Yanning , Zhang, Hongwei , Cai, Zhenping et al. Mesoporous polymer supported Metal-Based deep eutectic solvents for enhanced capture of Low-Content Ammonia . | CHEMICAL ENGINEERING JOURNAL , 2024 , 493 . |
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Carbon materials are commonly integrated with TiO2 to achieve high carrier mobility and excellent photocatalytic performance, and the chemical bond between TiO2 - C is considered as a significant strategy to enhance efficiency. Nevertheless, few analyses have elucidated the formation mechanism of Ti3+ - C bonds and the underlying reasons for the performance enhancement. To address these issues, this study conducts an in-depth investigation into the electronic structure of TiO2 - C and demonstrates that the charge in the nonbonding molecular orbital t2g of Ti3+ is transferred to the unoccupied 2p energy level of C through the formation of 1 pi and 2 pi bonds, i.e., (Ti 3d(xz) - C 2p(y)) and (Ti3d(xy) - C 2p(x)). The hybridization of t(2g)-2p orbitals endows the Ti3+ - C bond with higher carrier mobility and a stronger binding force, thereby contributing to stable photocatalytic H-2 production. Inspired by this scenario, the NSTiO2/rGO hybrid architecture, featuring the {101}/{001} surface heterojunction and the Ti3+ - C interfacial chemical bond, has been constructed. As a result, the hybrid catalyst exhibited excellent photocatalytic cycling stability of 92.9% and an H-2 evolution rate of 33.4 mmolh(-1)g(-1). This work proposes a strategy for designing efficient photocatalyst by regulating orbitals to achieve high-performance photocatalytic methanol splitting.
Keyword ：
cycling stability cycling stability photocatalytic methanol splitting photocatalytic methanol splitting surface heterojunction surface heterojunction t(2g)-2p orbital modulation t(2g)-2p orbital modulation Ti3+ - C chemical bond Ti3+ - C chemical bond
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| GB/T 7714 | Yu, Wen-Bei , Zhang, Heng-Rui , Zhang, Hong-Wei et al. Modulating Ti t2g Orbital Bonding in Dual-Channeled TiO2/rGO Hybrid Architecture for Stable Photocatalytic Methanol to Hydrogen [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (52) . |
| MLA | Yu, Wen-Bei et al. "Modulating Ti t2g Orbital Bonding in Dual-Channeled TiO2/rGO Hybrid Architecture for Stable Photocatalytic Methanol to Hydrogen" . | ADVANCED FUNCTIONAL MATERIALS 34 . 52 (2024) . |
| APA | Yu, Wen-Bei , Zhang, Heng-Rui , Zhang, Hong-Wei , Liu, Yao , Li, Yu , Su, Bao-Lian . Modulating Ti t2g Orbital Bonding in Dual-Channeled TiO2/rGO Hybrid Architecture for Stable Photocatalytic Methanol to Hydrogen . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (52) . |
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Aqueous-phase hydrogenation holds significance in achieving the large-scale green production of succinic acid, but the acidic reaction environment poses a considerable challenge in the design of highly active and stable catalysts. Herein, we report a spatial-confinement strategy to fabricate a Co-NPs@Co-N-C core-shell structured catalyst where Co nanoparticles (Co-NPs) are encapsulated tightly by nitrogen-doped graphitic carbon shells (NG), while Co single atoms (Co-SA) are distributed homogeneously on the shells, which exhibits remarkable efficiency and stability in the aqueous-phase hydrogenation of maleic acid for the production of succinic acid in an acidic medium. The catalyst achieves 100% conversion of maleic acid, more than 98% selectivity toward succinic acid, and high stability for seven cycles without significant deactivation. The combined characterizations and density functional theory (DFT) calculations further indicate that Co-NP and Co-SA can concurrently optimize the electronic structure of the NG and promote hydrogen dissociation on the surface of the carbon shells. These findings shed light on the unique function of Co-NP-NG-Co-SA composite sites on regulating the hydrogenation active centers and provide a guideline for the further development of highly efficient acid-resistant hydrogenation catalysts.
Keyword ：
acid-resistantcatalyst acid-resistantcatalyst aqueous phase hydrogenation aqueous phase hydrogenation composite active sites composite active sites core-shell structured catalyst core-shell structured catalyst succinic acid succinic acid
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| GB/T 7714 | Zhao, Zhengyu , Yang, Zongxuan , Bai, Hongmei et al. Highly Acid-Resistant CoNPs@Co-N-C Catalyst for the Efficient Aqueous-Phase Hydrogenation of Maleic Acid to Succinic Acid [J]. | ACS CATALYSIS , 2024 , 14 (20) : 15140-15149 . |
| MLA | Zhao, Zhengyu et al. "Highly Acid-Resistant CoNPs@Co-N-C Catalyst for the Efficient Aqueous-Phase Hydrogenation of Maleic Acid to Succinic Acid" . | ACS CATALYSIS 14 . 20 (2024) : 15140-15149 . |
| APA | Zhao, Zhengyu , Yang, Zongxuan , Bai, Hongmei , Zhang, Hongwei , Zhang, Bowen , Wu, Xinru et al. Highly Acid-Resistant CoNPs@Co-N-C Catalyst for the Efficient Aqueous-Phase Hydrogenation of Maleic Acid to Succinic Acid . | ACS CATALYSIS , 2024 , 14 (20) , 15140-15149 . |
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Heteroatom-incorporated zeolite catalysts are critical for biomass utilization and feedstock valorization in green chemistry. Key features are adjustable acidity, high stability, and a tailored range of functionalities. However, an environmentally benign synthesis of zeolites with good crystallinity and especially with high levels of metal substitution into the lattice remains challenging. Here, we propose a mechanochemistry-based liquid-assisted method (MCLA) for Zr-incorporated Beta zeolites that is high yielding, facile and sustainable. Compared with the fluoride-mediated hydrothermal method, crystallization times were considerably shortened so that Si-Beta and Zr-Beta (Si/Zr 100) zeolites can be synthesized within 9 and 15 h, respectively. Using the MCLA route, Beta zeolites with Zr loading up to 10.4 wt% (Si/Zr 12.5) were obtained. The materials have excellent catalytic activity for Meerwein-Ponndorf-Verley reductions with much higher water tolerance compared to Zr-Beta prepared by the post-synthesis method. The hydrophobic nature of the MCLA-synthesized zeolites makes them particularly useful as catalysts for organic reactions.
Keyword ：
Catalysis Catalysis Hydrophobicity Hydrophobicity Mechanochemistry Mechanochemistry Meerwein-Ponndorf-Verley reduction Meerwein-Ponndorf-Verley reduction Zr -Beta zeolites Zr -Beta zeolites
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| GB/T 7714 | Zhang, Hongwei , Jaenicke, Stephan , Okumura, Kazu et al. Mechanochemistry-based liquid-assisted synthesis of hydrophobic Zr-Beta with high metal loading for Meerwein-Ponndorf-Verley reduction [J]. | JOURNAL OF CATALYSIS , 2024 , 431 . |
| MLA | Zhang, Hongwei et al. "Mechanochemistry-based liquid-assisted synthesis of hydrophobic Zr-Beta with high metal loading for Meerwein-Ponndorf-Verley reduction" . | JOURNAL OF CATALYSIS 431 (2024) . |
| APA | Zhang, Hongwei , Jaenicke, Stephan , Okumura, Kazu , Tan, Hui-Ru , Chuah, Gaik-Khuan . Mechanochemistry-based liquid-assisted synthesis of hydrophobic Zr-Beta with high metal loading for Meerwein-Ponndorf-Verley reduction . | JOURNAL OF CATALYSIS , 2024 , 431 . |
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Defect-rich Pd/TiO2 catalysts are intensively adopted in heterogeneous hydrogenation reactions; however, the complexity of the defect structure makes it difficult to precisely identify which Pd-defect combination dominates the catalytic activity. Herein, defective TiO2 nanoflakes with tunable ratios of Vo to Ti3+ defects were synthesized and used to construct Pd-Vo and Pd-Ti3+ active sites after loading Pd to investigate the role of defects in regulating the structural and catalytic properties of defective Pd/TiO2 catalysts. Combining the experimental results and theoretical calculations, we reveal that both Vo and Ti3+ defects act as the electron donors for Pd and induce the strong metal-support interaction. When compared to the Vo defect, the Ti3+ defect behaves more significantly and donates more electrons, causing the Pd species on the catalysts to be better dispersed and more rich in electrons. These unique features endow the Pd-Ti3+ active centers with enhanced adsorption-activation ability toward C & boxH;C and H-2 as well as reduced energy barrier of the rate-limiting step, thus improving the intrinsic activity. The Pd-Ti3+ site manifests a high turnover frequency of 348 h(-1) and hydrogenation degree of 97% for hydrogenation of C & boxH;C in styrene-butadiene-styrene, which significantly outperforms the Pd-Vo site (254 h(-1) and 78%) and Pd nanoparticle (217 h(-1) and 53%). This work provides deep insight into the role of defects in regulating the properties of metal active sites, which can be used to guide the development of high-performance Pd/TiO2 catalysts for versatile applications.
Keyword ：
defective TiO2 defective TiO2 electronic structure electronic structure hydrogenation hydrogenation styrene-butadiene-styrene styrene-butadiene-styrene Ti3+-Pd site Ti3+-Pd site Vo-Pd site Vo-Pd site
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| GB/T 7714 | Wang, Shidong , Ge, Bingqing , Yang, Zongxuan et al. Construction of Highly Active Pd-Ti3+ Sites in Defective Pd/TiO2 Catalysts for Efficient Hydrogenation of Styrene-Butadiene-Styrene [J]. | ACS CATALYSIS , 2024 , 14 (3) : 1432-1442 . |
| MLA | Wang, Shidong et al. "Construction of Highly Active Pd-Ti3+ Sites in Defective Pd/TiO2 Catalysts for Efficient Hydrogenation of Styrene-Butadiene-Styrene" . | ACS CATALYSIS 14 . 3 (2024) : 1432-1442 . |
| APA | Wang, Shidong , Ge, Bingqing , Yang, Zongxuan , Zhang, Hongwei , Yang, Qin , Hu, Cejun et al. Construction of Highly Active Pd-Ti3+ Sites in Defective Pd/TiO2 Catalysts for Efficient Hydrogenation of Styrene-Butadiene-Styrene . | ACS CATALYSIS , 2024 , 14 (3) , 1432-1442 . |
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The efficient deoxygenation of renewable biolipids into liquid alkanes within the diesel range is a key protocol for producing high-quality biofuels. In this work, the conversion of methyl palmitate and raw palm oil were accomplished utilizing a bifunctional catalyst of Ni catalysts supported on B2O3-ZrO2 under solvent-free conditions. Among various Ni loading ratios investigated, the catalyst featuring a 10 % Ni loading achieved 100 % conversion of methyl palmitate and 84.4 % of liquid yield, with approximately 65 % being C15 alkanes. Additionally, more than 91 % of hydrocarbons were also generated from raw palm oil. These results can be attributed to the synergistic interplay between the acid sites, following B2O3 modification, and the presence of Ni species. Furthermore, the analysis of product distribution, gas product detection and the kinetics calculation strongly supports that the deoxygenation process of methyl palmitate primarily follows the hydrodecarbonylation route, leading to the predominant formation of C15 alkane.
Keyword ：
Bifunctional catalyst Bifunctional catalyst Biodiesel Biodiesel Deoxygenation Deoxygenation Liquid alkanes Liquid alkanes Methyl palmitate Methyl palmitate
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| GB/T 7714 | Yu, Panjie , Xu, Jing , Liang, Rengan et al. Solvent-free deoxygenation of biolipid into liquid alkanes over bifunctional Ni/B2O3-ZrO2 catalyst [J]. | FUEL , 2024 , 375 . |
| MLA | Yu, Panjie et al. "Solvent-free deoxygenation of biolipid into liquid alkanes over bifunctional Ni/B2O3-ZrO2 catalyst" . | FUEL 375 (2024) . |
| APA | Yu, Panjie , Xu, Jing , Liang, Rengan , Cai, Zhenping , Ma, Yongde , Zhang, Hongwei et al. Solvent-free deoxygenation of biolipid into liquid alkanes over bifunctional Ni/B2O3-ZrO2 catalyst . | FUEL , 2024 , 375 . |
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Electrocatalytic nitrate reduction reaction (NO3RR) has been capturing immense interest in the industrial application of ammonia synthesis, and it involves complex reaction routes accompanied by multi-electron transfer, thus causing a challenge to achieve high efficiency for catalysts. Herein, we customized the Cu-O-Ti-Ov (oxygen vacancy) structure on the Cu/TiO2 catalyst, identified through density functional theory (DFT) calculations as the synergic active site for NO3RR. It is found that Cu-O-Ti-Ov site facilitates the adsorption/association of NOx- and promotes the hydrogenation of NO3- to NH3 via adsorbed *H species. This effectively suppresses the competing hydrogen evolution reaction (HER) and exhibits a lower reaction energy barrier for NO3RR, with the reaction pathways: NO3* -> NO2* -> HONO* -> NO* -> *NOH -> *N -> *NH -> *NH2 -> *NH3 -> NH3. The optimized Cu/TiO2 catalyst with rich Cu-O-Ti-Ov sites achieves an NH3 yield rate of 3046.5 mu g h-1 mgcat-1 at -1.0 V vs. RHE, outperforming most of the reported activities. Furthermore, the construction of Cu-O-Ti-Ov sites significantly mitigates the leaching of Cu species, enhancing the stability of the Cu/TiO2 catalyst. Additionally, a mechanistic study, using in situ characterizations and various comparative experiments, further confirms the strong synergy between Cu, Ti, and Ov sites, which is consistent with previous DFT calculations. This study provides a new strategy for designing efficient and stable electrocatalysts in the field of ammonia synthesis. Published by Elsevier B.V. All rights reserved.
Keyword ：
Ammonia synthesis Ammonia synthesis Cu-O-Ti-O v site Cu-O-Ti-O v site Cu/TiO 2 catalyst Cu/TiO 2 catalyst Electrocatalytic nitrate reduction Electrocatalytic nitrate reduction Synergic catalytic effect Synergic catalytic effect
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| GB/T 7714 | Nie, Yifei , Yan, Hongping , Lu, Suwei et al. Theory-guided construction of Cu-O-Ti-Ov active sites on Cu/TiO2 catalysts for efficient electrocatalytic nitrate reduction [J]. | CHINESE JOURNAL OF CATALYSIS , 2024 , 59 : 293-302 . |
| MLA | Nie, Yifei et al. "Theory-guided construction of Cu-O-Ti-Ov active sites on Cu/TiO2 catalysts for efficient electrocatalytic nitrate reduction" . | CHINESE JOURNAL OF CATALYSIS 59 (2024) : 293-302 . |
| APA | Nie, Yifei , Yan, Hongping , Lu, Suwei , Zhang, Hongwei , Qi, Tingting , Liang, Shijing et al. Theory-guided construction of Cu-O-Ti-Ov active sites on Cu/TiO2 catalysts for efficient electrocatalytic nitrate reduction . | CHINESE JOURNAL OF CATALYSIS , 2024 , 59 , 293-302 . |
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Electrocatalytic oxidation as a promising route to produce value-added products from biomass-derived organics has received increasing attention in recent years. However, the efficient conversion of concentrated feedstock solutions with high selectivity and Faradaic efficiency (FE) remains challenging. Herein, we report a cation-defective Ni-based electrocatalyst derived from the surface reconstruction of the NiCo Prussian blue analogue (NiCo PBA) in alkaline media for the efficient oxidation of biomass-derived organics in a high concentration solution. Taking 5-hydroxymethylfurfural (HMF) as an example, the NiCo PBA can deliver a satisfactory catalytic performance in terms of high HMF conversion (97%), selectivity to 2,5-furandicarboxylic acid (98%), and FE (100%), even at a concentration as high as 100 mM. Theoretical calculations suggest that the cation defects not only promote the fast conversion of Ni(OH)(2) to electrochemically active NiOOH under anodic potential but also enhance the adsorption of HMF onto the active sites and accelerate the spontaneous chemical oxidation. This study provides deep insights into the structural evolution of PBA-based catalysts and reveals the pivotal factor that affects the performance of electrocatalytic oxidation, paving the way to further develop advanced electrocatalysts for efficient oxidation reactions with a high concentration.
Keyword ：
biomass upgrade biomass upgrade cation defects cation defects electrooxidation electrooxidation operandoRaman spectroscopies operandoRaman spectroscopies Prussian blue analogues catalysts Prussian blue analogues catalysts
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| GB/T 7714 | Zhang, Hongwei , Yang, Qin , Luo, Shuting et al. On the Activity and Selectivity of 5-Hydroxymethylfurfural Electrocatalytic Oxidation over Cation-Defective Nickel Hydroxides [J]. | ACS CATALYSIS , 2024 , 14 (12) : 9565-9574 . |
| MLA | Zhang, Hongwei et al. "On the Activity and Selectivity of 5-Hydroxymethylfurfural Electrocatalytic Oxidation over Cation-Defective Nickel Hydroxides" . | ACS CATALYSIS 14 . 12 (2024) : 9565-9574 . |
| APA | Zhang, Hongwei , Yang, Qin , Luo, Shuting , Liu, Zhichen , Huang, Jinming , Zheng, Yun et al. On the Activity and Selectivity of 5-Hydroxymethylfurfural Electrocatalytic Oxidation over Cation-Defective Nickel Hydroxides . | ACS CATALYSIS , 2024 , 14 (12) , 9565-9574 . |
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The electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) represents a promising pathway for producing biomass-derived value-added chemicals. Nevertheless, the use of extremely expensive ion exchange membranes (IEMs) as separators significantly sacrifices the economic benefit in large-scale applications. Herein, we report a cost-effective non-fluorine cation exchange membrane (CEM) by grafting sulfonic acid (-SO3- ) groups onto the aromatic side chain of the polyethersulfone (PES) polymer. By tuning the content of -SO3 - groups, the physicochemical properties of the resulting CEMs can be easily adjusted. Impressively, the optimal HBS-PES-1.0 CEM with fully grafted -SO3- groups can achieve a high HMF conversion of 100 %, FDCA selectivity of 98.0 %, and Faradaic efficiency of 98.3 % when used as the separator for electrocatalytic oxidation of HMF, surpassing that of the commercial Nafion 117 membrane (100 % HMF conversion, 98.1 % FDCA selectivity, and 97.4 % Faradaic efficiency). This study provides a cost-effective and high-performance CEM as a substitute for the expensive commercial membrane, paving the way to large-scale commercial applications of biomass upgrading through the electrolysis process.
Keyword ：
Biomass upgrading Biomass upgrading Cation exchange membrane Cation exchange membrane HMF electrocatalytic oxidation HMF electrocatalytic oxidation Side -chain type Side -chain type
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| GB/T 7714 | Zhang, Hongwei , Xu, Hao , Zhu, Zhen et al. Construction of non-fluorine side-chain cation exchange membranes for efficient 5-hydroxymethylfurfural electrocatalytic oxidation [J]. | JOURNAL OF MEMBRANE SCIENCE , 2024 , 706 . |
| MLA | Zhang, Hongwei et al. "Construction of non-fluorine side-chain cation exchange membranes for efficient 5-hydroxymethylfurfural electrocatalytic oxidation" . | JOURNAL OF MEMBRANE SCIENCE 706 (2024) . |
| APA | Zhang, Hongwei , Xu, Hao , Zhu, Zhen , Huang, Jinming , Zhang, Bowen , Cheng, Yafei et al. Construction of non-fluorine side-chain cation exchange membranes for efficient 5-hydroxymethylfurfural electrocatalytic oxidation . | JOURNAL OF MEMBRANE SCIENCE , 2024 , 706 . |
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The design of novel practical catalysts is critical for the blossoming of biodiesel green-energy, in which Mo-based catalysts are of particular interest. In this work, an in-situ synthesis method was proposed to obtain a combo Mo-based ionic liquid and SAPO-11 catalyst. The catalyst presents both highly dispersed MoS2 as hydrodeoxygenation active sites and acidic sites for isomerization. MoS2 with a few fine layers can be identified based on TEM images and the Bronsted acid sites are dominant based on Pyridine-IR analysis. A great performance of MoS2/C(8)min-15 %SA can be obtained under optimized reaction conditions with 100 % conversion of methyl palmitate, 75.0 mol% hydrodeoxygenation to n-C-15-C-16, and 20.5 mol % isomerization to i-C-15-C-16. The structure and activity of the catalyst can be retained at least for 4 cycles. Thin layers and high sulfurization, large amount of Br & oslash;nsted acid sites, and suitable reaction conditions are key points to achieve a significant performance and avoid over cracking and deactivation. On basis of detected intermediates and kinetic data simulations, a complex reaction pathway was proposed and the specific k values for each elementary reaction were provided for the hydrodeoxygenation and isomerization of methyl palmitate.
Keyword ：
Biodiesel Biodiesel Hydrodeoxygenation Hydrodeoxygenation Isomerization Isomerization Methyl palmitate Methyl palmitate MoS2 MoS2 SAPO-11 SAPO-11
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| GB/T 7714 | Ding, Yongxin , Lin, Jun , Yu, Panjie et al. An in-situ combo Mo-based ionic liquid and SAPO-11 catalyst for efficient biolipids hydrodeoxygenation and isomerization [J]. | FUEL , 2024 , 362 . |
| MLA | Ding, Yongxin et al. "An in-situ combo Mo-based ionic liquid and SAPO-11 catalyst for efficient biolipids hydrodeoxygenation and isomerization" . | FUEL 362 (2024) . |
| APA | Ding, Yongxin , Lin, Jun , Yu, Panjie , Zhang, Hongwei , Ma, Yongde , Cai, Zhenping et al. An in-situ combo Mo-based ionic liquid and SAPO-11 catalyst for efficient biolipids hydrodeoxygenation and isomerization . | FUEL , 2024 , 362 . |
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