ADVANCED MATERIALS
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2025
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IF 26.8
Zailun Liu,Yunfei Ma,Junqing Li,Ying Tu,Hui Yang,Kelin He,Chao Chen,Yulin Wang,Xiang Lin,Hongli Sun,Chenliang Su,Qitao Zhang
Uncovering the excitation processes of photocatalysts and enhancing the dissociation of excitons into free photogenerated electrons and holes for photocatalytic CO 2 reduction is imperative yet quite challenging. Herein, an efficient strategy of reducing the binding energy of excitons to boost exciton dissociation is reported by anchoring the low valence single-atom Cu sites in In 2 S 3 nanosheets (Cu-In 2 S 3 ), which can enhance photocatalytic CO 2 reduction activity. The investigations of photo-irradiated Kelvin probe force microscopy (KPFM), in situ irradiates X-ray photoelectron spectroscopy (XPS), and temperature-dependent photoluminescence (TD-PL) indicate that the doping of low valence single-atom Cu can efficiently drive the charge transfer and separation. Moreover, the studies of the dynamic behaviors of charge carriers by femtosecond time-resolved spectroscopy (fs-TAS) reveal that the doping of low valence Cu single-atom sites allows the promotion of exciton dissociation by reducing the binding energy of the exciton, resulting in an enhanced photocatalytic CO 2 reduction of Cu-In 2 S 3 nanosheets. The aforementioned strategy for enhancing the dissociation efficiency of excitons in photocatalysts will offer a highly efficient and promising approach for the photocatalytic CO 2 reduction and other photocatalytic applications.
研究领域:
光催化
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材料科学
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纳米技术
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物理化学
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能量转换
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产品关联
DOI
PubMed
高影响因子
ChemCatChem
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2025
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IF 3.9
Tianao Zhang,Haolong Huang,Yunchong Wang,Qianqian Zhao,Rui Han,Qingling Liu
Graphical CoO x /BCN catalyst with dual active sites was successfully synthesized. This catalyst exhibits excellent selectivity (99%) and a cyclic carbonate yield (98%) in the CO 2 cycloaddition reaction with the nucleophilic reagent KI under solvent-free and mild reaction conditions. This catalyst also has good stability and reusability, providing a new direction for the design of high-performance CO 2 cycloaddition catalysts. The carbon dioxide (CO 2 ) cycloaddition reaction provides an efficient route to achieve resource utilization of CO 2 . However, the inherent chemical stability of CO 2 itself hinders its efficient transformation into cyclic carbonates. Herein, the CoO x /BCN catalyst was successfully prepared by a simple deposition method. The CoO x /BCN exhibited excellent catalytic performance in the CO 2 cycloaddition reaction synergistically catalyzed with the nucleophilic reagent KI under solvent-free and mild reaction conditions (80 °C, 0.8 MPa, 6 h). The yield of cyclic carbonate was 98% and the selectivity was 99%, which was significantly superior to CoO x /CN catalyst (with a cyclic carbonate yield of 73.7%). Furthermore, after six cyclic reactions, CoO x /BCN still maintained a yield of over 93%. It was found that after boron (B) was doped into graphitic carbon nitride (g-C 3 N 4 ), the generated ─NB(OH) 2 group on CoO x /BCN effectively activated the epoxide. Importantly, the interaction between B-doped g-C 3 N 4 and CoO x induced the generation of abundant oxygen vacancies, which provided sufficient active sites for CO 2 adsorption and activation. In addition, carbonates were identified as the main reaction intermediates by in situ DRIFTS, and the possible reaction pathways of the CoO x /BCN catalyst were proposed. Therefore, this work provides new idea for the design of catalysts for CO 2 cycloaddition.
研究领域:
催化
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二氧化碳利用
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材料科学
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化学反应工程
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环境化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Keda Chen,Qinglan Tang,Lei Ran,Yifan Xu,Yongfa Zhu,Yizhen Zhang,Michael K.H. Leung
Solar-driven photocatalytic CO₂ conversion represents an innovative and eco-friendly approach to transform the predominant greenhouse gas into renewable fuels. Nevertheless, the slow movement of electron-hole pairs significantly restricts its wider practical applications. To address the challenge, our study investigates into the underlying mechanisms of the built-in electric field microenvironment, with the aim of elucidating its role in the electron transfer process. With synergistic effects stemming from its three-dimensional cross-linked porous structure and special charge-transfer pathway, triazine-based covalent organic frameworks (Tr-COFs, hereinafter referred to as COFs) were precisely anchored on lanthanum ferrate (LaFeO 3 ), forming LaFeO 3 /COFs (LFO/COF) Z -scheme heterojunction. The LFO/COF photocatalysts exhibited excellent visible light responsive performance for CO 2 reduction by achieving a high CO generation rate of 276.2 μmol g −1 h −1 with a CO selectivity of 94.4 %, significantly outperforming LaFeO 3 and COFs alone. The significant enhancement in photocatalytic CO₂ conversion can be ascribed to the build-in electric field of the Z -scheme heterojunction, which promotes efficient charge separation. Additionally, the porous structure of LFO/COF facilitated adsorption of CO 2 and desorption of CO. The reaction path of CO 2 → *CO 2 → *COOH→ *CO → CO. These results demonstrate that the interfacial electric field microenvironment is crucial for enhancing charge separation in the LFO/COF Z -scheme heterojunction, which enables efficient photocatalytic CO 2 reduction.
研究领域:
材料科学
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环境科学
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化学工程
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纳米技术
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物理化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Jingwei Li,Jianrui Feng,Xiaomin Guo,Hongli Fang,Jiayi Chen,Churong Ma,Ruchun Li,Yuya Wang,Zebao Rui
This work reports a novel strategy to activate type III heterojunction through introducing defect sites at the interfaces and making use of the defect band as the bridge for storage, secondary excitation, and interband transfer of the photothermal induced charges for constructing two-component Type B heterojunction photothermocatalyst. Type III heterojunction WO 3−x /GdCrO 3 is activated by defect-band state W 5/4+ at WO 3−x interface under photothermal conditions, achieving efficient charge separation, high redox potential, and full visible light absorption. The as-bridged (or Type B) heterojunction WO 3−x -R/GdCrO 3 as non-noble metal catalyst demonstrates excellent photothermocatalytic performance in toluene degradation with a reaction rate five times higher than that of WO 3−x /GdCrO 3 with less interfacial defect sites as well as in CO 2 reduction with high CO and CH 4 yielding rates of 49.6 μmol g −1 h −1 and 18.5 μmol g −1 h −1 in gas-solid reaction system without sacrifice agent, evidently better than those reported in the literature.
研究领域:
材料科学
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催化
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环境科学
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化学
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
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2021
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IF 9.127
Changfan Xu,Huanwei Wang,Jing Zhan,Yao Kang,Feng Liang
Designing catalytic cathodes with excellent electrocatalytic activities and durability for Na-CO 2 batteries has captured considerable attention so far. Here, a series of morphologically controlled low-crystalline CuCo 2 O 4 was prepared by thermal oxidation of self-assembled Cu-Co precursors ( p -CCO). One-dimensional (1D) rod-like of CuCo 2 O 4 was subsequently encapsulated in polypyrrole shell (PPy) by in-situ polymerization of pyrrole monomers as an advanced catalyst (CCO/PPy) for high-performance Na-CO 2 batteries . It was demonstrated that ammonia solution exerts an important influence on the surface morphology and size of the p -CCO crystallites by the rate of nucleation and growth. Particle size and 1D architecture modulation, associated with the encapsulation of conductive PPy effectively improve the directional transfer rate of ions and the conductivity of the electrode. More importantly, PPy introduction not only induces interfacial reconstruction of CuCo 2 O 4 , arousing more oxygen vacancies and catalytic active sites, but also contributes to the corrosion protection of the active material from the electrolyte during long-term operation. Bestowed by these advantages, the fabricated hybrid Na-CO 2 battery manifested prominent electrochemical performance with a superior areal discharge capacity of 31.3 mAh cm −2 , low discharge-charge voltage gap of 0.6 V, over 400 cycles.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
DOI
高影响因子
FOOD CHEMISTRY
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2025
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IF 9.8
Cong Jiang,Zong Meng
The development of green and efficient catalytic systems is crucial for sustainable chemical processes. This study engineered shellac nanoparticle-lipase conjugates for biphasic biocatalysis. Taking advantage of the inherent amphiphilicity and pH-triggered interfacial behavior of the shellac, the conjugates exhibited dual functionality as intelligent Pickering emulsifiers and interfacial biocatalysts. The covalent conjugation strategy achieved a protein loading capacity of 107.97 ± 5.24 mg/g under optimized conditions while preserving interfacial responsiveness. Reversible emulsification/breaking transitions were precisely regulated at least 30 times through pH adjustment or alternating CO₂/N₂ treatments, enabling convenient catalyst recovery. When applied to the esterification of phytosterols with oleic acid, the conjugates exhibited a higher esterification rate (78.93 %, 1.5-fold enhancement compared with the free lipase), retained 85.0 % initial catalytic activity after six consecutive cycles. The responsive Pickering system combined exceptional recyclability and enhanced catalytic performance, providing an innovative pathway for the development of Pickering interfacial catalysis.
研究领域:
绿色化学
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生物催化
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纳米技术
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胶体与界面科学
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酶工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED MATERIALS
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2025
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IF 26.8
Dashuai Li,Qi Wu,Changhua Wang,Zhehao Sun,Yingying Li,Zongyou Yin,Yichun Liu,Xintong Zhang
Transition metal high-entropy alloys (HEAs) demonstrate exceptional catalytic performance due to their structural complexity, featuring rich local atomic configurations, tunable electronic structures, and abundant active sites. However, this structural versatility poses both thermodynamic and kinetic challenges to conventional wet-chemical synthesis routes. Herein, we develop a novel solution plasma strategy that enables the direct synthesis of HEA catalysts in aqueous media. Through the FeCoNiCrMn electrode discharge in pure water, uniform HEAs nanoparticles (≈200 nm) are successfully anchored onto a variety of oxide substrates. The HEAs/TiO 2 catalyst achieves a CO generation rate of 298.1 mmol/g HEAs /h, representing ca. an order-of-magnitude higher activity than single-metal catalysts under both thermocatalytic and photothermal conditions. Advanced structural characterization reveals a dual-phase core-shell architecture consisting of a metallic alloy core and surface oxides preferentially enriched at CrMn sites. This spatially resolved structure enables cooperative catalysis, where CrMn-rich oxide domains promote H 2 dissociation, CoNi metallic regions facilitate CO 2 reduction, and Fe sites present in mixed valence states serve as electron and oxygen transfer bridges. We further identify a self-limiting oxidation mechanism intrinsic to plasma synthesis, which ensures charge redistribution at the metal-oxide interfaces and synergistically enhances photothermal catalysis. This work establishes an energy-efficient synthetic route for HEAs and elucidates structure-function relationships critical for advancing multimetallic catalytic systems.
研究领域:
材料科学
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催化
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纳米技术
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等离子体化学
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能量转换
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
AICHE JOURNAL
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2025
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IF 4
Fei Fan,Dechao Wang,Zengyi Li,Wulong Lu,Jianwei Liu,Xiaoyi Wei,Xu Cheng,Houxiang Sun,Huabing Zhang,Zhiping Chen,Wenwu Zhou
Developing high-performance supported non-precious metal copper-base catalysts for CO 2 hydrogenation is of extreme significance for the successful production of green methanol (CH 3 OH). Herein, Cu/ n Ge-CeO x catalysts ( n = 0, 0.25, 0.5, and 1 wt%) were synthesized via the incipient wetness impregnation method and comprehensively investigated using experiments and DFT calculations. Among all the catalysts, the Cu/0.5Ge-CeO x catalyst exhibited the highest concentration of oxygen vacancies, the smallest Cu grain size, and the most favorable regions for CO 2 adsorption. Compared to the Cu/0Ge-CeO x catalyst, the CH 3 OH yield was significantly improved over the Cu/0.5Ge-CeO x catalyst in the temperature range of 220–260°C under 3 MPa and a gas hourly space velocity of 3000 mL·g cat −1 ·h −1 . Especially at 260°C, the yield sharply increased from 35.23% to 82.21%, and this catalyst maintained high activity for 100 h. This was because the inert pair effect of the introduced Ge promoters induced lattice distortion on the support surface and regulated its microregion electron structures, while simultaneously establishing a highly active interface on the adjacent Cu cluster. This not only enabled an integrated process of in situ activated CO 2 and hydrogenation, but also inhibited the HCOO pathway, lowered the barrier of the rate-controlling step of the RWGS pathway, and reconciled some of its competing branching routes.
研究领域:
催化
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材料科学
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环境化学
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化学工程
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计算化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Chongyan Chen,Shuguang Shen,Jie Wang,Xingting Guo,Lili Zhang,Yongmei Liu,Jing Li
Replacing the oxygen evolution reaction (OER) with small molecule oxidation coupled with CO 2 reduction reaction (CO 2 RR) has become an effective strategy to reduce the energy demand of electrolyzers. However, the inconsistency of the cathode and anode products caused additional separation costs. Therefore, the selection of anodic paired-reactions capable of directing the same product is a key measure to solve the problem. At the same time, this poses a challenge for the design of bifunctional electrodes suitable for redox coupling systems. Herein, we established a coupled system in which the glucose oxidation reaction (GOR) is paired with the formate production via CO 2 RR, and for the first time, we have calculated its advantages through thermodynamic analysis. Additionally, a Sn 76.8 Co 23.2 electrode featuring crystalline Sn/amorphous SnCo heterointerfaces was prepared utilizing a revolutionary one-step in-situ electrodeposition method. It was demonstrated that the abundant two-phase interfaces optimized the redistribution of electrons, and that electrons transfer from Sn atoms to Co atoms to favor the adsorption of oxygen-containing intermediates, thereby improving the catalytic capability of Sn 76.8 Co 23.2 in the CO 2 RR, GOR semi-reaction, and CO 2 RR//GOR coupled system. This work provides invaluable insights into the matching of reactants and products for co-electrolysis systems, as well as a meaningful idea for the design of bifunctional electrocatalysts.
研究领域:
电化学
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材料科学
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催化
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能量转换
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2021
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IF 5.876
Jingke Song,Zhe Zhang,Songsong Zhi,Bingxuan Niu,Han Dong,Dapeng Wu,Kai Jiang
Background Development of human society has led to various environmental problems and energy crisis. Methods In this paper, Bismuth oxychloride (BiOCl) with a 3D network structure was prepared via a simple one-step sodium dodecylbenzenesulfonate (SDBS) assisted hydrothermal method and used for CO 2 reduction and antibiotic degradation. Consideration was given to the influence of addition of SDBS in the preparation process on the microscopic morphology and energy band structure of the photocatalyst. Significant findings The results of the present study indicate that the formation of the 3D network structure helps to expose the {001} facets of BiOCl and promotes the generation of more oxygen vacancies. As-prepared BiOCl-0.6, i.e., 0.78 g of Bi(NO 3 ) 3 ·5H 2 O with 0.6 g SDBS, demonstrating the highest photocatalytic reduction performance of CO 2 . The production of CO by BiOCl-0.6 can reach 59.5 and 20.1 µmol g −1 after 4 h of UV-vis/vis illumination, which is ten times higher than the control BiOCl. In addition, BiOCl prepared with a 3D network structure also showed efficient antibiotic (oxytetracycline hydrochloride, OTC) degradation ability. When the initial concentration of OTC was 20 mg/L, OTC was completely removed after 45 min of UV-vis irradiation, and 77.2% of OTC was removed after 90 min of photocatalytic reaction under visible light. In the photodegradation process, photogenerated holes (h + ) and superoxide radical ( · O 2 − ) play an important role.
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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光催化
✓ 已验证
DOI
高影响因子
Small Structures
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2025
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IF 11.3
Jiaojiao Fan,Jianmin Chen,Wenji Li,Zhongxing Zhao,Zhenxia Zhao
Converting CO 2 into high-value-added products via “artificial photosynthesis” under mild conditions is a promising yet challenging strategy for developing efficient photocatalysts. This study reports a simple two-step solvothermal approach to fabricate the dual-metal–organic framework (MOF) nanocomposite NH 2 -UiO-66@PCN-224 (NU-66@PCN-224) with tightly integrated interfaces, which achieves efficient CO 2 to CO photocatalytic reduction under light irradiation. The epitaxially grown PCN-224, composed of Zr 6 clusters and tetrakis (4-carboxyphenyl) porphyrin (TCPP), serves as a shell layer and a visible light-absorbing antenna, thereby broadening the light absorption range of the composite material. Moreover, the tightly integrated interfaces of NU-66@PCN-224 enhance the mobility of photogenerated charge carriers, consequently enhancing its capability for CO 2 catalytic reduction. As a result, the combination of NU-66 and PCN-224 retains their individual advantages while achieving a synergistic enhancement of both adsorption and catalysis, further improving the photocatalytic performance. The as-prepared NU-66@PCN-224 catalyst exhibits outstanding photocatalytic performance, yielding 74.6 μmol g −1 h −1 of CO under irradiation without sacrificial agents or photosensitizers. This work demonstrates a straightforward and effective method for designing MOF-on-MOF photocatalysts with enhanced photoactivity.
研究领域:
材料科学
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纳米技术
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环境科学
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光催化
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能量转换
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Xiaohua Jing,Jianying Huang,Jiani Shi,Zihan Zhao,Jingbo Hao,Xiaoning Tang
In this study, five novel ionic liquids (ILs), namely [N888][Cyanex 272], [N888][P507], [N888][Cl], [N888][NO3], and [N888]2[SO4], were synthesized through an organic acid–base reaction, followed by separation using rotary evaporation. Their structures were confirmed by 1H and 13C NMR spectroscopy, showing full consistency with theoretical predictions and no impurity peaks. Under identical extraction conditions, the ILs exhibited the following separation efficiency order for Co2+ from Ni2+: [N888]2[SO4]>[N888][Cl] > [N888][P507] > [N888][Cyanex 272]>[N888] [NO3]. Density functional theory (DFT) calculations revealed that these differences in separation performance arose from variations in the ionic radii of the IL anions. With a simple single-stage extraction under optimized conditions, [N888]2[SO4] enabled near-complete separation of Co2+ from Ni2+, achieving an extraction efficiency of 99.5 ± 2.14% and a separation factor approaching + ∞. Thermodynamic analysis confirmed that the extraction process was endothermic and nonspontaneous. The Co2+ -loaded IL-based extraction phase was efficiently stripped using diluted sulfuric acid, with a stripping efficiency of 99.3 ± 0.57%. Using sodium hydroxide as a precipitant, the solid powder of Co(OH)2 was obtained from the Co2+-containing aqueous phase. Co(OH)2 was characterized qualitatively and quantitatively by XRD and ICP-OES, and its morphology was also analyzed using SEM. The recycled IL-based extraction phase, after activation with dilute sulfuric acid, was analyzed via FT-IR spectroscopy. This regenerated IL-based extraction phase was reused for the separation of Co2+ from Ni2+, showing no degradation in performance after three cycles. Based on these findings, a process flowchart was designed for the efficient preparation of Co(OH)2 from minerals or secondary resources using the [N888]2[SO4]-based extraction phase.
研究领域:
化学工程
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材料科学
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环境科学
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无机化学
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分离技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）