Advanced Science
·
2023
·Vol. 10
·期 22
·2301869
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IF 15.1
Zhiyong Jiang,Xiaodi Zhu,Zhiyu Wang,Wei Liu,Wensheng Yan,Kevin Sivula,Jun Bao
The structural properties of octahedral sites (B Oh ) in spinel oxides (AB 2 O 4 ) play vital roles in the electrochemical performance of oxygen-related reactions. However, the precise manipulation of AB 2 O 4 remains challenging due to the complexity of their crystal structure. Here, a simple and versatile molten-salt-mediated strategy is reported to introduce Ni 2+ in B oh sites intentionally on the surface of zinc ferrite (ZnFe 2 O 4 , ZFO) to promote the active sites for photoelectrochemical (PEC) water splitting. The as-created photoanode (ZFO-MSNi) shows a remarkable cathodic shift of ≈ 450 mV (turn-on voltage of ≈ 0.6 V RHE ) as well as three times the 1-sun photocurrent density at 1.23 V RHE for PEC water oxidation in comparison with bare ZFO. A comprehensive structural characterization clearly reveals the local structure of the introduced Ni 2+ in ZFO-MSNi. Fewer surface trapping states are observed while the precisely introduced Ni 2+ and associated neighboring Fe (3- σ )+ (0< σ <1) sites unite in an edge-sharing octahedral configuration to function as Ni Fe dual active sites for PEC water oxidation. Moreover, open circuit potential measurements and rapid-scan voltammetry investigation give further insight into the enhanced PEC performance. Overall, this work displays a versatile strategy to regulate the surface active sites of photoelectrodes for increasing performance in PEC solar energy conversion systems.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Kexin Zhu,Fuping Zeng,Zhihui Li,Langlang Lv,Hua Jiang,Guangzhi Chen,Xiangyu Wang,Ju Tang
In this study, CuO-ZnO has been found to decompose sulfur hexafluoride (SF 6 ) with the activity higher than pure metal oxides (e.g. Al 2 O 3 ). After using the organic metal nanocage ZIF-8 as a precursor, the resulting CuO-ZnO particles exhibit uniform nanoscale size and possess an excellent surface area. When these particles are mixed with CaO and reacted with SF 6 at 600 °C and 0.2 MPa, a high SF 6 conversion rate of up to 99 % is achieved, with SO 2 making up about 98 % of the sulfur-containing products. Besides, the reaction demonstrates excellent degradation efficiency and maintains good stability over a continuous 78-hour operation. The results indicate that the CuO-ZnO particles provide abundant active sites that promote SF 6 adsorption and bond cleavage. Meanwhile, CaO helps disperse the CuO-ZnO particles, inhibits sintering, and provides an oxygen source for SO 2 formation, while also facilitating the fixation of fluorine, thereby enhancing both the selectivity and stability of the reaction. In addition, we also found that NH 3 is more conducive to promoting the decomposition of SF 6 by CuO-ZnO, whereas O 2 inhibits the progression of this reaction. Considering the global warming potential and long-term environmental impact of SF 6 , the proposed approach shows high degradation efficiency, excellent stability, and selectivity, contributing to mitigating the negative impact of SF 6 on global climate change.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
TALANTA
·
2024
·
IF 5.6
Huimin Yang,Yazhou Yang,Chaofan Ma,Qirui Wu,Jiahong Tang,Chaoqi Zhu,Xiaoxia Wang,Dawen Zeng
NO 2 is a hazardous gas extremely harmful to the ecosystem and human health, so effective detection of NO 2 is critical. SnSe 2 is a promising candidate for gas sensors owing to its unique layered configuration that facilitates the diffusion of gas molecules. Here, ultrathin self–assembled nanoflowers F–SnSe 2 rich in defects were synthesized by a simple solvothermal method. It exhibits excellent gas sensing performances for NO 2 at room temperature (25 °C), with a high gas sensing response of 8.6 for 1 ppm NO 2 and a lower detection limit as low as 200 ppb, capable of sensitively detecting ppb–level NO 2 . DFT calculations revealed that the presence of Se vacancies assists the central Sn atoms to break through the shielding effect of the surface Se atoms and become exposed active sites. The higher reactivity leads to more charge transfer and higher adsorption energy , which strongly promoted the adsorption of NO 2 . This work verifies the important role of vacancies for the exposed active sites and provides new guidance for defect engineering to modulate the gas sensing performances of SnSe 2 .
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Guangjun Ji,Cunyao Li,Benhan Fan,Guoqing Wang,Zhao Sun,Miao Jiang,Lei Ma,Li Yan,Yunjie Ding
Rational designing the structure of catalysts is an effective but challenging way to optimize catalytic performance for target reaction, which is especially significative in the field of single site catalysts. In this work, a kind of single Rh catalysts for heterogeneous hydroformylation of olefins with CO 2 as substituted carbonyl sources was designed. By simply doping N sites surround Rh P active sites, Rh 1 /POPs-P&N were endowed with better catalytic performance even than homogeneous Rh P complex catalysts. Our study showed that the fine fabricated skeleton structure of Rh 1 /POPs-P&N could endow the N sites with function promotion effect on the adjacent Rh P active sites to different degrees. Consequently, the Rh 1 / m -POP-PPh 3 &PMPD, which formed more HRh(CO) 2 (P) 2 species during the reaction, exhibited the highest yield of aldehydes (conversion of 89 %, selectivity toward aldehydes of 87.1 %, l/b ratio of 13.1), good stability (5 recycling runs without activity loss) and extensive substrate applicability (12 kinds of olefins) in heterogeneous hydroformylation of olefins with CO 2 , surpassing all homogeneous and heterogeneous catalysts that only contain Rh P sites (Table 5). Multiple characterization techniques (EXAFS, STEM, in-situ FTIR etc. ) were employed to get insights into this effective strategy to rationally design efficient single site catalysts.
研究领域:
催化
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材料科学
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化学反应工程
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无机化学
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 5
·2335
·
IF 4.6
Hongquan Kang,Jianzhou Wu,Baohui Lou,Yue Wang,Yilin Zhao,Juanjuan Liu,Shihui Zou,Jie Fan
The rational regulation of catalyst active sites at atomic scale is a key approach to unveil the relationship between structure and catalytic performance. Herein, we reported a strategy for the controllable deposition of Bi on Pd nanocubes (Pd NCs) in the priority order from corners to edges and then to facets (Pd NCs@Bi). The spherical aberration-corrected scanning transmission electron microscopy (ac-STEM) results indicated that Bi2O3with an amorphous structure covers the specific sites of Pd NCs. When only the corners and edges of the Pd NCs were covered, the supported Pd NCs@Bi catalyst exhibited an optimal trade-off between high conversion and selectivity in the hydrogenation of acetylene to ethylene under ethylene-rich conditions (99.7% C2H2conversion and 94.3% C2H4selectivity at 170 °C) with remarkable long-term stability. According to the H2-TPR and C2H4-TPD measurements, the moderate hydrogen dissociation and the weak ethylene adsorption are responsible for this excellent catalytic performance. Following these results, the selectively Bi-deposited Pd nanoparticle catalysts showed incredible acetylene hydrogenation performance, which provides a feasible perspective to design and develop highly selective hydrogenation catalysts for industrial applications.Keywords:acetylene hydrogenation;active sites;selective deposition;palladium;bismuth
研究领域:
催化化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 22
·10857-10865
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IF 3.3
Jinglin Zhu,Meng Zhu,Juanjuan Peng
Developing highly active Fenton-like materials for the decontamination of water is a hot topic. Nanosized Fe3O4 particles are green catalysts for environmental remediation, but their application is limited by their low catalytic activity. Herein, Fe3O4 rhombic dodecahedral nanoparticles (Fe3O4-R) with exposed {110} facets were synthesized via the solvothermal method and used as a Fenton-like catalyst for the degradation of bisphenol A (BPA). Consequently, ∼100% of BPA was removed using Fe3O4-R/H2O2 at pH = 5.0, which was higher than that by commercial Fe3O4. Multiple experiments confirmed the presence of abundant Fe(II) active sites on the surface of Fe3O4-R, but they were unstable, resulting in the dissolution of Fe(II) from the solid surface via oxidation, and thus the homogeneous reaction was not negligible in the Fe3O4-R/H2O2 process. However, hydroxyl radicals (HO˙) were still the primary reactive species, playing a dominant role in the removal of BPA. Consequently, the degradation of BPA was easily disturbed by HCO3− and natural organic matter (NOM). Unfortunately, the inactivation of Fe3O4-R was observed in cycle experiments, which is ascribed to the stabilization of the surface of Fe3O4-R during the oxidation process, reducing the surface active sites of Fe(II). Therefore, this study provides new insight into the Fenton-like oxidation process for the degradation of pollutants by regulating the morphology of Fe3O4 nanoparticles.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
·
2025
·
IF 3.1
Peng Lu,Yuqi Peng,Xiaoxue Wang,Shiying Chen,Jing Shang,Shuyu Qi,Yue Yang,Xueli Hu,Zilong Zhao
To enhance the photocatalytic degradation performance of Bi 2 O 3 against tetracycline (TC) pollutants, a Biochar/Bi 2 O 3 (BC/Bi 2 O 3 ) composite photocatalyst was synthesized using chitin as a carbon source through a one-step calcination method. The tetracycline degradation efficiency of the photocatalytic material (m BC: Bi2O3 = 2:1) synthesized at 500 °C for 4 h was reached 83.43 %, as well as 5.5 and 1.5 times higher than that of the BC and Bi 2 O 3 monomers, respectively, while the degradation rate constant of BC/Bi 2 O 3 (2:1) was 0.0052 min −1 , which was 13 and 1.7 times higher than that of BC (0.0004 min −1 ) and Bi 2 O 3 (0.0030 min −1 ). Extensive property analysis shows that BC and Bi 2 O 3 interact through Bi-O-C bonds after synthesize, which improves the electron transport efficiency and provides more active sites for the composite. The interaction between these two materials allows the composite to provide more active sites while improving the electron transfer efficiency. UV–vis spectroscopy and free radical quenching experiments further corroborated the direct degradation ability of the BC/Bi 2 O 3 composite photocatalyst towards TC. As the reaction progressed, TC undergoes degradation mineralization via two distinct pathways, faciliatetd by the action of h + and •O 2 − radicals. Overall, the functional BC/Bi 2 O 3 with high photocatalytic activity provides worthwhile insights of photocatalytic materials application in the wasterwater treatment field.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2025
·
IF 6.3
Menghe Lou,Li Xiang,Guo Nie,Xueqing Luo,Renna Li,Feng Bi,Xiaole Weng,Zhongbiao Wu
The removal of carbon monoxide (CO) from sintering flue gases remains a significant challenge in industrial gas purification, requiring efficient catalytic systems. This study explores the use of TiO 2 synthesized under supercritical conditions in copper-based catalysts for low-temperature CO oxidation. Experimental results showed enhanced catalytic activity, with complete CO conversion at 120°C, primarily due to a higher Cu⁺ concentration in the catalyst. Characterization techniques (XPS, EPR, CO-DRIFT) confirmed a substantial increase in the Cu⁺ ratio in Cu/sc-TiO 2 (78%) compared to Cu/TiO 2 (71%) before thermal treatment. Additionally, the Cu/sc-TiO 2 -A catalyst exhibited smaller particle size and better dispersion, which contributed to the elevated Cu⁺ ratio after preheating. Thermal treatment increased the Cu⁺ ratio by 11% in Cu/sc-TiO 2 -A, compared to just 3% in Cu/TiO 2 -A, leading to a final Cu⁺ ratio of 89%, which enhanced catalytic activity. DRIFT and TPSR analyses indicated that the Cu/sc-TiO 2 catalyst generated CO during heat treatment, creating a micro-reduction environment that optimized copper valence states and active sites. This study highlights the potential of continuous hydrothermal flow synthesis for modulating catalyst valence states in industrial applications.
研究领域:
材料科学
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催化化学
·
环境工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 25
·e202304989
·
IF 1.9
Ying Chen,Zhangyi Lv,Jinqiu Yuan,Mingchun Bi,Yuning Liang
Graphical ZIF-67 nanocubes (ZIF-67 NCs) had been etched to produce small amounts of cross-linked Co-LDH-1 while preserving the cubic structure, which provided sufficient quantities of cobalt ions. The catalytic activity of OER has been enhanced by the cubic-structured LDH, which leads to a significantly lower overpotential in alkaline media and a calculated lower activation energy Ea. To address the substantial energy needs of the quickly evolving modern civilization, efforts are still needed to provide sustainable renewable energy sources. The electrocatalytic Oxygen evolution reaction (OER) is one of the essential technologies used in the various hydrogen production techniques. ZIF-67 nanocubes (ZIF-67 NCs) were synthesized in an aqueous solution and used as sacrificial templates. Cobalt nitrate hexahydrate was added under water bath conditions, resulting in the evolution of numerous small layered layers of cobalt hydroxide. This ultimately led to the formation of multilayered, three-dimensionally crosslinked Co-LDH with a porous networked cubic morphology. Hydrolysis of Co 2+ at different concentrations produces different degrees of weak acidic environments, and the loose LDH on the cubic structure of the best catalyst, Co-LDH-1, exposes more active cobalt sites for the OER, which results in a high electrochemically active surface area, with an overpotential of 354 mV and a Tafel slope of 79.06 mV dec −1 at a current density of 10 mA cm −2 , and good stability and low activation under alkaline condition also has good stability and low activation energy. It provides us an easy and practical plan for logically creating ZIF-derived hydroxide materials, leading to the development of affordable and effective electrocatalysts.
研究领域:
材料科学
·
电化学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Guojuan Hai,Jianfeng Huang,Liyun Cao,Koji Kajiyoshi,Long Wang,Liangliang Feng
Designing and synthesizing heterojunction electrocatalyst with abundant active sites is critical to optimize the activity of electrochemical water splitting. Herein, a typical hierarchical W 18 O 49 /NiWO 4 heterojunction grown on nickel foam was successfully synthesized via a multistep synthesis strategy. The electrochemical oxidation and reduction process triggers the amorphization of W 18 O 49 and significantly enhances the interfacial interaction, thereby endowing the composites with enriched active sites. The W 18 O 49 /NiWO 4 /NF is completely reconstructed to NiWO 4 /NF and NiWO 4 /NiOOH/NF with amorphous-crystalline interface (denoted as H-AM/NiWO 4 /NF for HER and O-AM/NiWO 4 /NiOOH/NF for OER). The valence of tungsten ions is well modulated to achieve a high proportion of tetravalent W (IV) active sites accompanied by abundant oxygen vacancies. The increased Ni (III) ions as OER active sites have strong orbital overlap with reaction intermediate, which stabilize the low-valent W (IV) by producing more NiOOH species during the oxygen evolution reaction. Benefiting from the amorphous–crystalline composites, unsaturated W (IV) sites, abundant oxygen vacancies, and highly active NiOOH species, the activated electrocatalyst exhibits excellent electrocatalytic activity, achieving a small overpotential of 1.53 V at 10 mA·cm −2 for water-splitting and maintaining long-term stability at least 100 h.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Zhengfeng Shen,Feifei Li,Jiangrui Lu,Zhidan Wang,Rui Li,Xiaochao Zhang,Changming Zhang,Yawen Wang,Yunfang Wang,Zhiping Lv,Jianxin Liu,Caimei Fan
Photocatalytic nitrogen fixation has been considered to be a safe, green, eco-friendly, and sustainable technology. However, photoinduced activation of inert dinitrogen is an important factor hindering the development of this technology. Herein, in-situ Fe 3+ doped flower-like BiOCl with highly active sites exposure was prepared by a solvent thermal method, which has excellent performance of N 2 photofixation. Compared with virgin BiOCl with no nitrogen fixation activity, Fe-BiOCl reached 30 μmol·L −1 ·h −1 ammonia evolution rate under simulated sunlight without any sacrificial reagent. Characterization results demonstrated that the enhancement of N 2 photofixation capacity was mainly attributed to the in-situ doped Fe 3+ in BiOCl, the doped Fe 3+ not only acts as a reaction center for N 2 activation also as an “electron transfer bridge” trapping and migrating electrons from BiOCl to N 2 molecules. Furthermore, the transformation of crystal facets from virgin BiOCl (0 0 1) to Fe-BiOCl (1 1 0) and (1 0 2) is more conducive for the exposure and accessibility of iron reactive sites. This work developed a potential strategy by in-situ introducing Fe 3+ active sites in BiOCl semiconductor substrate, which establishes a good basis for the application of semiconductor catalysts in nitrogen fixation.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Yiqing Zeng,Yanan Wang,Shule Zhang,Qin Zhong,Weilong Rong,Xiaohai Li
In this work, novel (CeO 2 ) x -(CePO 4 ) 1−x (defined as Ce x P 1−x ) nanorod composites were prepared by a simple co-precipitation method, and the influence of CeO 2 on the catalytic performance of CePO 4 for selective catalytic reduction of NO by NH 3 (NH 3 -SCR of NO) was investigated. The catalytic performance evaluation revealed that the Ce x P 1−x catalysts, especially Ce 0.2 P 0.8 exhibited a much better catalytic activity and H 2 O + SO 2 resistance than CePO 4 . Structure characterizations via high-resolution transmission electron microscope (HRTEM) and Brunauer-Emmett-Teller (BET) revealed that the introduction of CeO 2 had a little effect on the shape of CePO 4 nanorods and it could promote the formation of new mesoporous then significantly enhance the surface area of catalyst. The analysis results of active sites suggested that phosphorus was the main adsorption site for NH 3 and the redox sites were controlled by CeO 2 on Ce x P 1−x catalysts. Finally, reaction process study demonstrated that the NH 3 -SCR over Ce x P 1−x was processed via Langmuir-Hinshelwood (L-H) mechanism. Combining the results of active sites and reaction mechanism analysis, it was drawn that the superior low temperature activity of Ce x P 1−x could be attributed to its excellent redox properties, which promoted the oxidation of NO then facilitated the process of NH 3 -SCR via “fast SCR”.
研究领域:
材料科学
·
催化化学
✓ 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）