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学者姓名：胡策军
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Abstract ：
Water electrolysis for hydrogen production holds great promise as an energy conversion technology. The electrolysis process contains two necessary electrocatalytic reactions, one is the hydrogen evolution reaction (HER) at the cathode, and the other is the oxygen evolution reaction (OER) at the anode. In general, the kinetics of OER is much slower than that of HER, dominating the overall of performance electrolysis. As identified, the slow kinetics of catalytic OER is mainly resulted from multiple electron transfer steps, and the catalysts often undergo compositional, structural, and electronic changes during operation, leading to complicated dynamic reaction mechanisms which have not been fully understood. Obviously, this challenge presents formidable obstacles to the development of highly efficient OER electrocatalysts. To address the issue, it is crucial to unravel the origins of intrinsic OER activity and stability and elucidate the catalytic mechanisms across diverse catalyst materials. In this context, in-situ/operando characterization techniques would play a pivotal role in understanding the catalytic reaction mechanisms by enabling real-time monitoring of catalyst structures under operational conditions. These techniques can facilitate the identification of active sites for OER and provide essential insights into the types and quantities of key reaction intermediates. This comprehensive review explores various catalyst design and synthesis strategies aimed at enhancing the intrinsic OER activity and stability of catalysts and examines the application of advanced in-situ/operando techniques for probing catalyst mechanisms during the OER process. Furthermore, the imperative need for developing innovative in-situ/operando techniques, theoretical artificial intelligence and machine learning and conducting theoretical research to better understand catalyst structural evolution under conditions closely resembling practical OER working states is also deeply discussed. Those efforts should be able to lay the foundation for the improved fabrication of practical OER catalysts.
Keyword ：
Electrocatalysts Electrocatalysts In-situ techniques In-situ techniques Oxygen evolution reaction Oxygen evolution reaction Reaction mechanism Reaction mechanism
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| GB/T 7714 | Hu, Cejun , Hu, Yanfang , Zhang, Bowen et al. Advanced Catalyst Design Strategies and In-Situ Characterization Techniques for Enhancing Electrocatalytic Activity and Stability of Oxygen Evolution Reaction [J]. | ELECTROCHEMICAL ENERGY REVIEWS , 2024 , 7 (1) . |
| MLA | Hu, Cejun et al. "Advanced Catalyst Design Strategies and In-Situ Characterization Techniques for Enhancing Electrocatalytic Activity and Stability of Oxygen Evolution Reaction" . | ELECTROCHEMICAL ENERGY REVIEWS 7 . 1 (2024) . |
| APA | Hu, Cejun , Hu, Yanfang , Zhang, Bowen , Zhang, Hongwei , Bao, Xiaojun , Zhang, Jiujun et al. Advanced Catalyst Design Strategies and In-Situ Characterization Techniques for Enhancing Electrocatalytic Activity and Stability of Oxygen Evolution Reaction . | ELECTROCHEMICAL ENERGY REVIEWS , 2024 , 7 (1) . |
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Lignin is continuously investigated by various techniques for valorization due to its high content of oxygencontaining functional groups. Catalytic systems employing hydrolysis-hydrogenolysis, leveraging the synergistic effect of redox metal sites and acid sites, exhibit efficient degradation of lignin. The predominance of either hydrolysis or hydrogenolysis reactions hinges upon the relative activity of acid and metal sites, as well as the intensity of the reductive atmosphere. In this study, the Pd-MoOx/TiO2 catalyst was found to primarily catalyze hydrolysis in the lignin depolymerization process, attributed to the abundance of moderate acidic sites on Pd and the redox-assisted catalysis of MoOx under inert conditions. After subjecting the reaction to 240 degrees C for 30 h, a yield of 48.22 wt% of total phenolic monomers, with 5.90 wt% consisting of diphenols, was achieved. Investigation into the conversion of 4-propylguaiacol (4-PG), a major depolymerized monomer of corncob lignin, revealed the production of ketone intermediates, a phenomenon closely linked to the unique properties of MoOx. Dehydrogenation of the propyl is a key step in initiating the reaction, and 4-PG could be almost completely transformed, accompanied by an over 97 % of 4-propylcatechol selectivity. This distinctive system lays a new theoretical groundwork for the eco-friendly valorization of lignin.
Keyword ：
4-Propylguaiacol 4-Propylguaiacol Hydrogen-free Hydrogen-free Hydrogenolysis Hydrogenolysis Hydrolysis Hydrolysis Ketone Ketone Lignin Lignin
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| GB/T 7714 | Tang, Daobin , Lin, Xuebin , Zhang, Qi et al. Hydrolysis-dominated catalytic system: Hydrogen-free hydrogenolysis of lignin from Pd-MoO x /TiO 2 [J]. | INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES , 2024 , 267 . |
| MLA | Tang, Daobin et al. "Hydrolysis-dominated catalytic system: Hydrogen-free hydrogenolysis of lignin from Pd-MoO x /TiO 2" . | INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES 267 (2024) . |
| APA | Tang, Daobin , Lin, Xuebin , Zhang, Qi , Wang, Zhenni , Liu, Yuhang , Jin, Yanqiao et al. Hydrolysis-dominated catalytic system: Hydrogen-free hydrogenolysis of lignin from Pd-MoO x /TiO 2 . | INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES , 2024 , 267 . |
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Microfluidic synthesis has emerged as a promising method for synthesizing metal-organic frameworks (MOFs). It overcomes the limitations of the traditional solvothermal method to regulate the structure and function of the MOFs. This study synthesized various MOFs with different structures and functions by controlling the reaction time and the ratio of metal ions to organic ligands through microfluidics and investigated their CO2 adsorption properties. The results showed that the microfluidic synthesized defective and hierarchical pore MOF-808 improved the adsorption performance of CO2 by nearly 110% and 30%, respectively, compared with solvothermal synthesized MOF-808.
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| GB/T 7714 | Ge, Xuehui , Liu, Zihan , Wei, Nanjie et al. Microfluidic Synthesis of Defective and Hierarchical Pore Zr Metal-Organic Framework Materials and CO2 Adsorption Performance Study [J]. | CRYSTAL GROWTH & DESIGN , 2024 , 24 (21) : 9084-9096 . |
| MLA | Ge, Xuehui et al. "Microfluidic Synthesis of Defective and Hierarchical Pore Zr Metal-Organic Framework Materials and CO2 Adsorption Performance Study" . | CRYSTAL GROWTH & DESIGN 24 . 21 (2024) : 9084-9096 . |
| APA | Ge, Xuehui , Liu, Zihan , Wei, Nanjie , Lin, Xiaocheng , Hu, Cejun . Microfluidic Synthesis of Defective and Hierarchical Pore Zr Metal-Organic Framework Materials and CO2 Adsorption Performance Study . | CRYSTAL GROWTH & DESIGN , 2024 , 24 (21) , 9084-9096 . |
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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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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 electrocatalytic carbon dioxide or carbon monoxide reduction reaction (CO2RR or CORR) features a sustainable method for reducing carbon emissions and producing value-added chemicals. However, the generation of C3 products with higher energy density and market values, such as n-propanol, remains highly challenging, which is attributed to the unclear formation mechanism of C3+ versus C2 products. In this work, by the Tafel slope analysis, electrolyte pH correlation exploration, and the kinetic analysis of CO partial pressure fitting, it is identified that both n-propanol and C2 products share the same rate-determining step, which is the coupling of two C1 intermediates via the derivation of the Butler-Volmer equation. In addition, inspired by the mechanistic study, it is proposed that a high OH & horbar; concentration and a water-limited environment are beneficial for promoting the subsequent *C2-*C1 coupling to n-propanol. At 5.0 m [OH-], the partial current density of producing n-propanol (jn-propanol) reached 45 mA cm-2, which is 35 and 1.3 times higher than that at 0.01 m [OH-] and 1.0 m [OH-], respectively. This study provides a comprehensive kinetic analysis of n-propanol production and suggests opportunities for designing new catalytic systems for promoting the C3 production. A comprehensive kinetic analysis is conducted using the Butler-Volmer equation, including Tafel slopes, pH dependence, and the theoretical current density of n-propanol versus CO partial pressure, revealing *CO dimerization is the common rate-limiting step for both n-propanol and C2 products. A potential strategy is then used to promote the CO electroreduction performance to n-propanol. image
Keyword ：
Butler-Volmer equation Butler-Volmer equation electrochemical CO reduction electrochemical CO reduction electrokinetic analysis electrokinetic analysis n-propanol n-propanol rate-determining step rate-determining step
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| GB/T 7714 | Yan, Yaqin , Liu, Kunhao , Yang, Chao et al. Electrokinetic Analysis-Driven Promotion of Electrocatalytic CO Reduction to n-Propanol [J]. | SMALL , 2024 , 20 (50) . |
| MLA | Yan, Yaqin et al. "Electrokinetic Analysis-Driven Promotion of Electrocatalytic CO Reduction to n-Propanol" . | SMALL 20 . 50 (2024) . |
| APA | Yan, Yaqin , Liu, Kunhao , Yang, Chao , Chen, Yangshen , Lv, Ximeng , Hu, Cejun et al. Electrokinetic Analysis-Driven Promotion of Electrocatalytic CO Reduction to n-Propanol . | SMALL , 2024 , 20 (50) . |
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The electrocatalytic CO2 or CO reduction reaction is a complex proton-coupled electron transfer reaction, in which protons in the electrolyte have a critical effect on the surface adsorbed *H species and the multi-carbon oxygenate products such as ethanol. However, the coupling of *H and carbon-containing intermediates into C2+ oxygenates can be severely hampered by the inappropriate distributions of those species in the catalytic interfaces. In this work, the controlled distribution of highly dispersed CeOx nanoclusters is demonstrated on Cu nanosheets as an efficient CO electroreduction catalyst, with Faradaic efficiencies of ethanol and total oxygenates of 35% and 58%, respectively. The CeOx nanoclusters (2-5 nm) enabled efficient water dissociation and appropriate distribution of adsorbed *H species on the Cu surface with carbon-containing species, thus facilitating the generation of C2+ oxygenate products. In contrast, pristine Cu without CeOx tended to form ethylene, while the aggregated CeOx nanoparticles promoted the surface density of *H and subsequent H2 evolution.
Keyword ：
CeOx CeOx CO electrocatalysis CO electrocatalysis Faradaic efficiency Faradaic efficiency oxygenate product oxygenate product surface adsorbed *H surface adsorbed *H
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| GB/T 7714 | Yang, Chao , Yan, Yaqin , Hu, Yuncheng et al. Promoting CO Electroreduction to C2+ Oxygenates by Distribution of Water Dissociation Sites [J]. | SMALL METHODS , 2024 , 9 (1) . |
| MLA | Yang, Chao et al. "Promoting CO Electroreduction to C2+ Oxygenates by Distribution of Water Dissociation Sites" . | SMALL METHODS 9 . 1 (2024) . |
| APA | Yang, Chao , Yan, Yaqin , Hu, Yuncheng , Chen, Yangshen , Guan, Anxiang , Hu, Cejun et al. Promoting CO Electroreduction to C2+ Oxygenates by Distribution of Water Dissociation Sites . | SMALL METHODS , 2024 , 9 (1) . |
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In recent years, studies focusing on the conversion of renewable lignin-derived oxygenates (LDOs) have emphasized their potential as alternatives to fossil-based products. However, LDOs, existing as complex aromatic mixtures with diverse oxygen-containing functional groups, pose a challenge as they cannot be easily separated via distillation for direct utilization. A promising solution to this challenge lies in the efficient removal of oxygen-containing functional groups from LDOs through hydrodeoxygenation (HDO), aiming to yield biomass products with singular components. However, the high dissociation energy of the carbon–oxygen bond, coupled with its similarity to the hydrogenation energy of the benzene ring, creates a competition between deoxygenation and benzene ring hydrogenation. Considering hydrogen consumption and lignin properties, the preference is directed towards generating aromatic hydrocarbons rather than saturated components. Thus, the goal is to selectively remove oxygen-containing functional groups while preserving the benzene ring structure. Studies on LDOs conversion have indicated that the design of active components and optimization of reaction conditions play pivotal roles in achieving selective deoxygenation, but a summary of the correlation between these factors and the reaction mechanism is lacking. This review addresses this gap in knowledge by firstly summarizing the various reaction pathways for HDO of LDOs. It explores the impact of catalyst design strategies, including morphology modulation, elemental doping, and surface modification, on the adsorption–desorption dynamics between reactants and catalysts. Secondly, we delve into the application of advanced techniques such as spectroscopic techniques and computational modeling, aiding in uncovering the true active sites in HDO reactions and understanding the interaction of reactive reactants with catalyst surface-interfaces. Additionally, fundamental insights into selective deoxygenation obtained through these techniques are highlighted. Finally, we outline the challenges that lie ahead in the design of highly active and selective HDO catalysts. These challenges include the development of detection tools for reactive species with high activity at low concentrations, the study of reaction medium–catalyst interactions, and the development of theoretical models that more closely approximate real reaction situations. Addressing these challenges will pave the way for the development of efficient and selective HDO catalysts, thus advancing the field of renewable LDOs conversion. © 2024 Institute of Process Engineering, Chinese Academy of Sciences
Keyword ：
Catalyst design Catalyst design Hydrodeoxygenation Hydrodeoxygenation Lignin-derived oxygenates Lignin-derived oxygenates Targeted deoxidation Targeted deoxidation Techniques and theoretical calculation Techniques and theoretical calculation
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| GB/T 7714 | Wu, X. , Zhang, H. , Hu, C. et al. Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques [J]. | Green Energy and Environment , 2024 , 10 (2) : 292-321 . |
| MLA | Wu, X. et al. "Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques" . | Green Energy and Environment 10 . 2 (2024) : 292-321 . |
| APA | Wu, X. , Zhang, H. , Hu, C. , Bao, X. , Yuan, P. . Advances in enhancing hydrodeoxygenation selectivity of lignin-derived oxygenates: From synthetic strategies to fundamental techniques . | Green Energy and Environment , 2024 , 10 (2) , 292-321 . |
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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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Photocatalytic reduction of CO2 into syngas is a promising way to tackle the energy and environmental challenges; however, it remains a challenge to achieve reaction decoupling of CO2 reduction and water splitting. Therefore, efficient production of syngas with a suitable CO/H-2 ratio for Fischer-Tropsch synthesis can hardly be achieved. Herein, bipolaronic motifs including Co(II)-pyridine N motifs and Co(II)-imine N motifs are rationally designed into a crystalline imine-linked 1,10-phenanthroline-5,6-dione-based covalent organic framework (bp-Co-COF) with a triazine core. These featured structures with spatially separated active sites exhibit efficient photocatalytic performance toward CO2-to-syngas conversion with a suitable CO/H-2 ratio (1:1-1:3). The bipolaronic motifs enable a highly separated electron-hole state, whereby the Co(II)-pyridine N motifs tend to be the active sites for CO2 activation and accelerate the hydrogenation to form *COOH intermediates; whilst, the Co(II)-imine N motifs increase surface hydrophilicity for H-2 evolution. The photocatalytic reductions of CO2 and H2O thus decouple and proceed via a concerted way on the bipolaronic motifs of bp-Co-COF. The optimal bp-Co-COF photocatalyst achieves a high syngas evolution rate of 15.8 mmol g(-1) h(-1) with CO/H-2 ratio of 1:2, outperforming previously reported COF-based photocatalysts.
Keyword ：
bipolaronic construction bipolaronic construction charge separation and transfer charge separation and transfer covalent triazine frameworks covalent triazine frameworks photocatalytic reduction of CO2 photocatalytic reduction of CO2 syngas syngas
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| GB/T 7714 | Zhao, Chengfeng , Yang, Chao , Lv, Ximeng et al. Bipolaronic Motifs Induced Spatially Separated Catalytic Sites for Tunable Syngas Photosynthesis From CO2 [J]. | ADVANCED MATERIALS , 2024 , 36 (25) . |
| MLA | Zhao, Chengfeng et al. "Bipolaronic Motifs Induced Spatially Separated Catalytic Sites for Tunable Syngas Photosynthesis From CO2" . | ADVANCED MATERIALS 36 . 25 (2024) . |
| APA | Zhao, Chengfeng , Yang, Chao , Lv, Ximeng , Wang, Shengyao , Hu, Cejun , Zheng, Gengfeng et al. Bipolaronic Motifs Induced Spatially Separated Catalytic Sites for Tunable Syngas Photosynthesis From CO2 . | ADVANCED MATERIALS , 2024 , 36 (25) . |
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