Journal of Materials Chemistry A
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2025
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IF 9.5
Lang Pei,Haichuan Feng,Qinan Mao,Lixiang Wang,Yu Zhang,Xin Wen,Xusheng Wang,Xiao Liu
Efficient photocatalytic CO₂ reduction necessitates optimal charge balance and proton migration between the CO₂ reduction and H₂O oxidation half-reactions. However, traditional research has predominantly focused on optimizing these half-reactions independently, neglecting potential synergistic effects. Here, this work demonstrates a photothermal catalyst of Pt/Ta2O5-x nanoplates that synergistically leverages the photothermal effect and redox dual-site cooperation to simultaneously accelerate the CO₂ reduction and H₂O oxidation, thereby maximizing proton-electron transfer. The integration of photothermal effect and photocatalysis ensures a strong driving force for CO2 conversion while accelerating proton migration, with Pt plasmonics generating localized heat from solar energy. In-situ characterizations reveal that O vacancy in Ta2O5-x enhances H2O dissociation to provide abundant protons, while Pt acts as electron acceptor sites, effectively activating the C=O bond. Theoretical calculations further illustrate the synergistic CO2 reduction and H2O oxidation on Pt and O vacancy sites, where the oxidation of *OH to *OOH is synchronized with the *CO desorption to CO, significantly lowering the energy barrier for proton-coupled electron transfer. Impressively, the Pt/Ta2O5-x exhibits exceptional photothermal catalytic performance in CO2-to-syngas conversion with a syngas yield up to 1.97 mmol g⁻¹ h⁻¹, which is 16.3-fold higher than Ta2O5-x. Furthermore, the apparent quantum efficiency reaches 3.5% at 365 nm, and the syngas selectivity is a remarkable 82%, while also exhibiting good stability.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
Advanced Energy Materials
·
2020
·Vol. 10
·期 38
·2001592
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IF 25.245
Xiaodong Lin,Zongqiang Sun,Chun Tang,Yuhao Hong,Pan Xu,Xueyang Cui,Ruming Yuan,Zhiyou Zhou,Mingsen Zheng,Quanfeng Dong
The reduction of O 2 to solid Li 2 O 2 on discharge and the reverse oxidation of Li 2 O 2 to O 2 on recharge are the essential processes to determine the performance of Li-O 2 batteries. The discovery of effective catalysts with a favorable Li 2 O 2 formation/decomposition mechanism is vital for the development of high-performance Li-O 2 batteries. Here, a soluble catalyst of iodosylbenzene (PhIO) that can offer a highly reversible O 2 conversion is reported for the first time. Benefiting from its ability to capture and couple the LiO 2 intermediate, which is endowed by its polarized I 3+ O 2− bond where the I atom and O atom can serve as a Lewis acidic site and basic site (dual site) to interact with O 2 − and Li + , respectively, the formation and decomposition of Li 2 O 2 by a one-electron pathway can be effectively promoted, thus greatly improving the electrode surface passivation issue and the reaction kinetics. In addition, the side reactions caused by the traditional high-reactive LiO 2 intermediate can also be effectively suppressed by forming a series of low-reactive intermediates (LiO 2 3PhIO, (LiO 2 ) 2 4PhIO, and Li 2 O 2 4PhIO) instead. Consequently, the PhIO-catalyzed Li–O 2 batteries exhibit a low overpotential, a large capacity, and a good cyclability.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Qiaoyu Zhang,Chengcheng Chen,Fangting Liu,Zhengguo Zhang,Xiaoming Fang,Qiong Liu
The in-situ photocatalytic selective reduction of O 2 to produce H 2 O 2 is a promising green and sustainable production technique. However, it faces significant challenges due to the high reaction energy barrier of the H 2 O oxidation half-reaction, which inhibits the reaction and leads to undesirable oxidative by-products. In this study, we have the first time developed a O/Cs dual-functional carbon nitride material for the simultaneous photocatalytic reduction of O 2 to synthesize H 2 O 2 and the selective oxidation of xylose to produce xylonic acid. The CN-O/Cs material exhibits excellent photocatalytic activity for H 2 O 2 production at 820.6 μmolh −1 (41.03 mmolh -1 g −1 ), while achieving a xylose oxidation rate of 359.5 μmolh −1 to xylonic acid, surpassing most reported catalytic systems and enabling biomass upgrading. It is elucidated that the introduction of Cs atoms serves as new reduction active sites, significantly enhancing the adsorption of O 2 with the transitioning Pauling type adsorption configuration. And the Cs atoms facilitate the deprotonation capability of H 2 O to form the crucial *OOH while lowering the reaction energy barrier. The presence of oxygen atoms plays a role in redistribution of electron density, and promotes the selective oxidation of the aldehyde group at the edge of xylose. The synergistic functionalities of Cs and O atoms enable the efficient utilization of electron-hole pairs for the simultaneous synthesis of H 2 O 2 and xylonic acid. This study demonstrates that the rational design of multifunctional tandem sites materials at the atomic scale for the synergistic synthesis of H 2 O 2 and selective oxidation of biomass holds promising prospects.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
RARE METALS
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2025
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IF 11
Luo Qi-Zhi,Huang Jin-Shu,Liu Teng-Yu,Yuan Ji-Li,Belousov Artem S.,Li Sheng-Kun,Yang Song,Li Hu
Photocatalytic selective synthesis of lactic acid (LA) from biomass sugars with a single heterogeneous catalyst is promising but challenging due to the multiple reaction steps involved. Herein, a K-doped C-rich red polymerized carbon nitride (RPCN) photocatalyst with uniform K/C dual sites was constructed by a molten salt template method, which was highly efficient for cascade isomerization dehydration of glucose to LA with > 90% selectivity under visible light and gentle conditions. Control experiments and theoretical calculations expounded that the introduced K/C dual sites could improve the light capture ability and photogenerated charge separation efficiency, while the K species provided sufficient Lewis acid sites (adsorption sites) for the isomerization of glucose to fructose. Meanwhile, the introduced C sites that substitute N atoms could promote electrons to be captured by adsorbed oxygen for selective generation of superoxide radicals, which was highly efficient for the scission of the C3–C4 bond in fructose, exclusively furnishing LA. Importantly, the RPCN photocatalyst was also suitable for the photocatalytic upgrading of various biomass saccharides into LA with high yields of 81.3%–95.3% and could be recycled for five consecutive cycles. The tailored construction of dual sites by localization of space charge lightens an avenue for multi-step conversion of biomass with pronounced selectivity. Graphical abstract
研究领域:
催化化学
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可再生资源转化
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2021
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IF 8.742
Long Tian,Nigel Graham,Ting Liu,Kening Sun,Wenzheng Yu
Two-dimensional (2D) graphene oxide (GO) membranes continue to attract interest due to their superior permeation and separation performance, and are regarded as a promising technology for water purification . However, the imperfect interlayer microstructure under the applied hydraulic pressure, and the inferior stability are still considerable challenges to achieve high permeability, selectivity and operability. In this paper, we describe for the first time, the development and testing of a dual-site supported GO membrane (SEN-Mg/GO) by introducing biuret (SEN) and Mg 2+ inside the interlayer structure. SEN can support the GO sheets in the oxide sites based on a condensation reaction between amino and carboxyl groups, while Mg 2+ is fixed in the graphitic sites through a non-covalent cation-π interaction. A synergistic effect of the dual-site crosslinking and support build more favorable nanochannels for the rapid transport of water while also imparting the membrane to maintain a tightly-packed 2D structure, which increases water flux without sacrificing the separation performance. In comparison, SEN-Mg/GO exhibited a water flux 4 times greater than the GO and SEN only cross-linked GO membrane (SEN/GO), with high selectivity towards various model dye molecules (>98%). The SEN-Mg/GO membrane also achieved greater “trade-off” between flux and rejection and significantly improved stability than the Mg 2+ only cross-linked GO membranes (Mg/GO). The optimized nanochannels and the interlayer covalent bond are considered to be the dominant factors in improving the separation performance and stability of the membrane, respectively. The dual-site supporting technique provides a new approach for the fabrication of GO membranes of high performance, and can be used in the design of other 2D lamellar membranes.
研究领域:
材料科学
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环境工程
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膜技术
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Jiang Mo,Su Liu,Quan-Qing Xu,Xiang-Ying He,Wei-Hua Mu,Ming-Yu Teng,Wen-Fu Fu
In this work, Pt single atoms (SAs) were engineered on the surface of CdIn 2 S 4 (CIS) to trigger abundant generation and stable existence of sulfur vacancies (S v ). Through quasi in situ X-ray photoelectron spectroscopy (XPS) and work function analysis, the photogenerated electrons are first captured by Pt SAs and S v , and then transferred from Pt SAs to S v , ultimately increasing the electron density of S v . Meanwhile, S v have significant advantages in adsorbing CO 2 molecules. According to the number of transferred electrons, the optimized 0.8 %Pt/CIS has 76 times the photocatalytic performance of pristine CIS, and the selectivity of ethylene (C 2 H 4 ) is up to 99.3 %. The carbon–carbon coupling reaction between *CO and *CHO adsorbed on double sites of S v and In atoms is identified as the rate-determining step. Theoretical calculations suggest that the energy barrier required for coupling of intermediates *CO and *CHO is the lowest, conducive to the selective generation of C 2 H 4 .
研究领域:
材料科学
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环境科学
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催化化学
✓ 已验证
DOI
高影响因子
ACS Nano
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2025
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IF 16
Shuo Meng,Shanshan Yang,Ting He,Jian Guo,Mingze Xu,Lu Chen,Kexuan Liao,Lianhai Zu,Chen Zhou,Chi Zhang,Jinhu Yang
Benzoquinone (BQ) is considered a promising cathode material for aqueous zinc-ion batteries due to its simplest molecular structure and highest theoretical specific capacity among quinones. However, intrinsic problems derived from BQ including severe dissolution, narrow crystal interplanar d-spacings accessible by desolved Zn2+ only, and poor conductivity cause inferior battery performance. Herein, a strategy based on a “nanopore-confined dual-site synergy mechanism” is proposed to stabilize the BQ cathode and boost Zn2+ desolvation/coordination reactions for stable and fast Zn storage, which is realized by the construction of CoS2 nanodot-embedded MOF-derived porous carbon (MPC) as an efficient host for BQ molecules. The MPC provides enough pore space to accommodate a substantial amount of BQ molecules with good electric conductivity, whereas CoS2 in pores offering abundant Co and S sites exerts strong chemical binding over BQ species and facilitates Zn2+ desolvation/coordination, respectively, synergistically suppressing the dissolution of cathodes and imparting the rapid reaction kinetics of batteries. Consequently, the developed BQ@CoS2-MPC cathode delivers a high reversible capacity of 458 mA h g–1 at 0.5 C, excellent rate capability, and pronounced cycling stability with a low decay of 0.003% per cycle for over 10,000 cycles at 20 C. The work proposes an effective strategy toward high-performance organic electrode materials.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
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2025
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IF 13.1
Yifan Li,Jiaxing Li,Lin Chen,Yunpeng Long,Xing Yuan,Junhua Li,Yue Peng
The low selectivity for N2 in the oxidation of NH3 over commercial Pt/Al2O3 catalysts is primarily due to the overoxidation of NH3 facilitated by Pt sites, leading to the formation of unwanted byproducts such as N2O and NO. In this study, we present a novel strategy to enhance N2 selectivity while maintaining NH3 conversion by constructing Pt–O–Cu dual sites. These dual sites exhibit synergistic acid-redox characteristics through surface electron transfer mediated by bridged lattice oxygen. Additionally, the ability of surface-adsorbed oxygen to exchange with lattice oxygen is significantly improved. The electron-deficient Cu sites enhance NH3 adsorption by providing empty 3d orbitals, while the electron-rich Pt sites promote NH3 dehydrogenation. Subsequently, the formation of –NH or –N intermediates at the Pt sites can react with adsorbed NH3 on the Cu sites to produce N2, predominantly following the integrated selective catalytic reduction mechanism. The optimized dual-site catalyst achieves over 95% NH3 conversion and N2 selectivity at 180 °C.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Dou Zhang,Ying-jie Sun,Kai-hua Zhang,Guang Yang,Xiao-jing Wang,Yi-lei Li,Hui-yun Han,Xinying Liu,Bao-Hang Han,Fa-tang Li
Synchronizing the directional photogenerated transfer of electrons and regulating the CO 2 photocatalytic reduction process are key to achieving the efficient and highly selective photocatalytic reduction of CO 2 . The design of highly-dispersed active sites and the efficient collaboration of multiple sites are of great importance in attaining the above target. Herein, a reverse etching route was first proposed to confine Bi single atoms and nanoparticles as dual-sites for assisting CO 2 photoreduction on TiO 2 , avoiding the mutual masking of the active sites. The Synergism of the dual-sites achieves the hydrodeoxygenation of * COOH and ushers the directional conversion of CO 2 to CH 4 . Highly dispersed single Bi atoms could induce the transfer of photogenerated electrons, enhance CO 2 absorption, and further provide active sites for reducing CO 2 to *COOH intermediates. Besides, appropriate Bi nanoparticles could promote the separation and transfer of photogenerated and inhibit the formation of hydroxyl groups; more importantly, they could promote the release of protons, which would further accelerate the conversion of *COOH to CH 4 . After being integrated, the optimized dual-Bi/TiO 2 catalyst achieves a CH 4 generation rate of 103.89 μmol·g −1 ·h −1 with an impressive selectivity of 96.87 % as well as remarkable durability for photocatalytic CO 2 reduction. This work provides new insights into developing robust catalysts through the artful design of synergistic catalytic sites for efficient photocatalytic CO 2 conversion.
研究领域:
材料科学
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催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
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2024
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IF 14
Hongqiang Yang,Jianfeng Zheng,Guoyu Wang,Yifei Gao,Yatao Yang,Jia Li,Xiaojin Han,Yan Cui,Zhanggen Huang
Photoelectrocatalytic coupling CO 2 and volatile organic compounds (VOCs) is a promising green strategy for the synergistic conversion of the two carbon-containing resources to C 2 products. The catalytic efficiency is always at the mercy of chemical inertness of CO 2 and the competitive hydrogen evolution of H 2 O. Herein, a modified g-C 3 N 4 /ZnAl-LDH Z-scheme heterojunction catalyst with dual reaction site was rationally designed and precisely constructed. The Faraday efficiency of ethanol reached 68.67% with a corresponding formation rate of 227.3 μmol g −1 h −1 . As revealed by in-situ characterizations and density functional theory calculations, CO 2 and HCHO were absorbed at Zn site and N site, respectively. Then, *CO generated from CO 2 and HCHO was converted to *CH 3 O and *CHO on the dual-active-site heterojunction. The detailed reaction mechanism experiments indicated that C–C coupling only occurred between *CO and *CH 3 O in electrocatalysis process. Apart from the “*CO + *CH 3 O” path, another “*CO + *CHO” coupling path was also detected in photoelectrocatalytic process. The selectivity of ethanol was significantly enhanced due to the synthesis of dual-site catalyst and the dual-path coupling path between CO 2 and HCHO simultaneously driven by light and electricity.
研究领域:
环境科学
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材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Zhicheng Xu,Yuran Li,Yuting Lin,Yan Wang,Qiang Wang,Tingyu Zhu
To strengthen the CO oxidation activity of activated carbon for flue gas purification, AC was modified through acid treatment and metal loading. AC-supported Cu shows excellent catalytic oxidation activity compared with other metal-modified AC samples. To investigate the action modes of Cu loaded on activated carbon and the mechanism of CO oxidation, various samples were characterized by XRD, N 2 O titration, SEM, N 2 physisorption, TPD, H 2 -TPR, XPS, in situ DRIFTS and EPR. The results show that oxygen-containing functional groups increase the loading amount and dispersion of Cu. Moreover, Cu species strongly bound to oxygen-containing functional groups are the main contributors to CO oxidation. The roles of oxygen-containing functional groups are further revealed: carboxyl groups are the anchoring sites of Cu, and hydroxyl groups supply oxygen to restore the active structure. Similarly, Ce indirectly promote the oxidation activity of CO by re-oxidizing Cu + to Cu 2+ , which accelerates the catalytic cycle. The reaction mechanism on AC-supported Cu samples has been proposed to follow the double-site Langmuir–Hinshelwood mechanism, with Cu 2+ as oxidation sites, Cu + as adsorption sites and the formation of oxygen vacancies on Cu + during the reaction. AC-Cu performs the highest oxidation activity at a proportion of Cu + of 0.5–0.6. SO 2 causes irreversible chemical poisoning to CO oxidation, while NO leads to reversible poisoning due to competitive adsorption with CO. The novel AC-supported Cu catalyst with Ce improves the resistance against SO 2 and NO, and the reason is explained. These findings provide theoretical guidance for the preparation and application of metal-modified activated carbon.
研究领域:
环境科学
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催化化学
✓ 已验证
DOI
高影响因子
TALANTA
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2017
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IF 4.162
Xiaoxiao Su,Mengyao Wang,Yue Wu,Yong He,Zhifeng Fu
A novel dual-site recognition protocol was developed for chemiluminescent (CL) detection of Streptococcus mutans ( S. mutans ) based on a designed antibiotic-affinity strategy. Teicoplanin , a broad-spectrum antibiotic against Gram-positive bacteria, was adopted to functionalize magnetic particles and recognize S. mutans utilizing the strong affinity between this agent and D-Alanyl-D-Alanine peptide moieties in the bacterial cell wall. To achieve ideal specificity for S. mutans detection, rat immunoglobulin G2a (rat IgG2a) tagged with horseradish peroxidase (HRP) was used as the second recognition agent and signal tracer since Fab region of rat IgG2a could bind with streptococcal protein G highly expressed in the cell wall of S. mutans . Thus HRP-tagged sandwich complex of teicoplanin/ S. mutans /rat IgG2a was formed on the magnetic particles, followed by a CL quantification of S. mutans based on a HRP-catalyzed luminol-H 2 O 2 -p -iodophenol CL reaction. This dual-site recognition protocol showed a linear range of 1.0 × 10 2 –1.0 × 10 6 CFU mL −1 and a detection limit of 33 CFU mL −1 for S. mutans detection. The whole detection process could be completed within 70 min. The recovery tests for food, environmental, pharmaceutical and biological samples showed acceptable recovery values between 83.0% and 110.0%, demonstrating its application potential for detection of bacteria in various sample matrixes.
研究领域:
微生物学
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分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）