CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yulong Xiang,Xinbin Ji,Xiaoli Dong,Yu Wang,Nan Zheng,Chundong Liu,Menglin Wang,Chumin Yan
Photoreduction of toxic Cr(VI) in wastewater to less toxic Cr(III) presents an effective approach to address the environmental issues. Nevertheless, the photocatalytic performance of these photocatalysts is severely constrained by their narrow light absorption range and the rapid recombination of photo-generated electrons and holes. Herein, DUT-67/Fe 2 O 3 heterojunction photocatalysts were prepared by a simple mechanical grinding method. The formation of DUT-67/Fe 2 O 3 heterostructures not only increased the specific surface area and light absorption range, but also improved the separation of photogenerated charge carriers. Compared to the pristine DUT-67, DUT-67/Fe 2 O 3 exhibited significantly improved photocatalytic performance in the reduction of Cr(VI), achieving a reduction efficiency of up to 94 % within 40 min. Active species trapping experiments identified that electrons served as the primary species in the photocatalytic process. Coupled with electron spin resonance and density functional theory (DFT) calculations, a comprehensive mechanism for the photocatalytic reduction of Cr(VI) by DUT-67/Fe 2 O 3 Z-scheme heterojunction was proposed. This work offers new insights into the underlying mechanisms involving in the interfacial charge transfer and Cr(VI) photoreduction processes.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 41
·32714-32719
·
IF 3.84
Gui-lin Zhuang,Jia-qi Bai,Li Tan,Hong-liang Huang,Yi-fen Gao,Xing Zhong,Chong-li Zhong,Jian-guo Wang
Zr-based MOFs usually feature exceptionally high thermal and chemical stability, which suggests that composites of noble metals and Zr-based MOFs could have wide industrial applications. In this work, we report the synthesis and characterization of Pd nanoparticles (of three different loadings: 0.3%, 0.5% and 1.0%) supported on micro-crystal DUT-67 MOFs. Via SEM, TEM and XPS characterization methods, it was found that the Pd nanoparticles were well dispersed on the interface of the MOF micro-crystals, with a diameter of 3.5 nm, and both the dangling organic groups and the cavities of the MOFs play important roles. Furthermore, PXRD, IR, TGA and N2 adsorption measurements confirmed that the composites are very robust. Studies on the catalytic properties indicated that they have good catalytic performance with a conversion of 99% and selectivity of 89% in the Suzuki coupling reaction. By a series of explorations, we found the best catalytic conditions are an ethanol–water mixed solvent as the medium, K2CO3 as the base and a temperature of 70 °C. Moreover, good catalytic properties were also shown for the hydrogenation of nitrobenzene, where the optimum temperature was 60 °C, and a conversion of 99% and selectivity of 99% were achieved.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Jinjing Qiu,Qi Chen,Cheng Liu,Yueling Chen,Jionghua Wu,Kaiqiang Jing,Jimmy C. Yu,Ling Wu,Xianzhi Fu
Defect engineering and single atom incorporation can provide more active sites to modulate the surface electronic structure of a catalyst and to activate reactant molecules. Herein, a series of Ru-anchored DUT-67(Zr) MOFs with explicit defect sites have been prepared for photocatalytic nitrogen reduction. It is characterized that Ru/DUT-67(Zr) possesses uniformly dispersed Ru single atoms and unsaturated Zr. Typically, 1.0 %Ru/DUT-67(Zr) shows best performance with a NH 4 + yield of 61.1 μmol·g −1 ·h −1 , which is approximately 6-folds higher than that of defective DUT-67(Zr) without Ru single atom (DUT-L), while pristine DUT-67(Zr) exhibits a lack of the photocatalytic N 2 reduction activity. The observed enhancement can be attributed to the introduction of Ru and unsaturated Zr sites induced by irradiation. Both of them can work together act as active centers to absorb and activate dinitrogen molecule. Furthermore, benefited from the electronic channel (Ru-S) between Ru and DUT-67(Zr), the separation of photogenerated carriers has been greatly improved, contributing to the collaborative conversion of activated N 2 to NH 3 . This study provides a new insight for designing a dual active sites photocatalyst with unsaturated coordinated sites and the single atoms by the coordinately interaction of functionalized linker.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Xiaoqin Wei,Hao Guo,Zongyan Lu,Lei Sun,Zhilan Pan,Bingqing Liu,Liping Peng,Wu Yang
Uric acid and dopamine are closely related to the health of the organism, so it is important to determine them simultaneously and efficiently. In this paper, the metal-organic framework DUT-67 was in situ grown on the surface of bimetallic oxide ZnCo 2 O 4 nanoflowers , and then ultrasonically compounded with multi-walled carbon nanotubes (MWCNTs) to prepare DUT-67/ZnCo 2 O 4 -MWCNTs composite. The prepared composite was characterized by XRD , SEM, XPS , FTIR, BET and other techniques. Finally, an electrochemical sensor based on DUT-67/ZnCo 2 O 4 -MWCNTs composite modified glassy carbon electrode for simultaneous detection of dopamine (DA) and uric acid (UA) was fabricated. The introduction of ZnCo 2 O 4 into the composite efficiently overcame the disadvantage of the easy aggregation of DUT-67 and produced a synergistic effect with MWCNTs. The electron transfer rate between the electrode and the electrolyte solution was accelerated, and the detection signals of the target molecules were amplified. After characterizing the electrochemical properties of the composite electrode, it was found that the constructed electrochemical sensor showed low detection limits for DA and UA, which were 12 nM and 8.7 nM, respectively, and the wide linear range of 1.0–180.0 μM. Besides, the sensor had excellent reproducibility, repeatability, anti-interference and stability. The proposed sensor was also successfully used to determine the contents of DA and UA in dopamine injection and urine samples with relatively satisfactory recovery rates. This work not only provides a new strategy for the preparation of MOF modified electrodes , but also has a potential application prospect in bioassays.
研究领域:
生物医学工程
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2019
·
IF 2.938
Wenke Li,Zhe Cai,Hang Li,Yu Shen,Yongqiang Zhu,Haichao Li,Xubin Zhang,Fumin Wang
One-pot conversion of furfural to the target product γ-valerolactone (GVL) is a challenging and meaningful part of biomass exploitation. Development of heterogeneous catalysts with both Brønsted and Lewis acid properties has proved to be promising and useful because they offer an efficient way to tandem cascade reactions from furfural to GVL. Herein, we successfully synthesized sulfated DUT-67(Hf), a novel bifunctional catalyst, via a post-synthetic modification method. The prepared sulfated DUT-67(Hf) was characterized by XRD, SEM, TEM, N 2 adsorption-desorption, Elemental (N, C, H, S) analyses, situ infrared spectra of pyridine adsorptions, XPS, FT-IR, TG, and NH 3 -TPD. The acidity of the catalysts could be adjusted by submersion in different concentrations of aqueous sulfuric acid, giving 0.01 mol/L sulfuric acid for 0.42 mmol/g acidity to 0.1 mol/L sulfuric acid for 2.16 mmol/g acidity. Sulfated DUT-67(Hf) possessed by 0.06 mol/L aqueous sulfuric acid exhibited optimal catalytic activity and showed an 87.1% yield of GVL under the conditions of 180 °C after 24 h of reaction. Moreover, the mechanism of introducing Brønsted acid sites into DUT-67(Hf) and the better hydrogen donors was also investigated through contrasting experiments.
研究领域:
化学工程
·
催化化学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2026
·
IF 17.2
Yun Huang,Qi Chen,Yueling Chen,Zefeng Yang,Jionghua Wu,Jimmy C. Yu,Ling Wu
The generation of active hydrogen species (H*) is an essential step in the photocatalytic conversion of nitrogen molecules (N 2 ) to ammonia (NH 3 ). Metal-organic frameworks (MOFs) are versatile porous structures but they do not exhibit sufficient photocatalytic activities for nitrogen fixation. Adding appropriate amounts of noble metal species as a cocatalyst to MOFs can often improve their activities. This work uses a photoreduction strategy to reduce the right amount of Pt 4+ to Pt clusters, and confines the remaining Pt 4+ uniformly onto DUT-67(Zr). This is realized by taking advantage of a unique Pt-S electron channel, and the unsaturated Zr sites are concurrently in-situ generated under light exposure. The unsaturated Zr sites adsorb and activate N 2 , while the Pt clusters are involved in the water splitting process on DUT-67(Zr) to generate more H*, leading to continuous H* supply that would speed up the catalytic hydrogenation of nitrogen intermediate NH x . The Pt-S electronic channel formed between highly dispersed single atoms Pt and DUT-67(Zr) facilitates the separation and transfer of photo-generated charge carriers. Consequently, with the synergistic effect of unsaturated Zr sites, Pt clusters and Pt-S electron channels, a high photocatalytic nitrogen fixation performance of 78.8 μmol g ‒1 h ‒1 can be achieved. This is 10.4 times higher than that of the sample DUT-67-L with only unsaturated Zr sites and no Pt loading. This work provides an insight to rational design of uniform dispersed precious metal-based MOF photocatalyst for efficient photocatalytic ammonia synthesis.
✓ 已验证
产品关联
DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2026
·
IF 3.3
Xiang Yulong,Ji Xinbin,Dong Xiaoli,Wang Yu,Zheng Nan,Luo Yang,Zhao Honglin,Yan Chumin
Charge separation, transfer, and recombination are crucial factors that influence the efficiency of photocatalytic Cr(VI) reduction. The construction of Schottky junctions can remarkably facilitate the spatial separation of charge carriers. To address the issue of heavy metal pollution in industrial wastewater, an Ag-DUT-67 Schottky junction photocatalyst was synthesized by depositing silver nanoparticles (Ag NPs) onto the DUT-67 surface through a photoreduction technique. The findings indicate that Ag NPs are evenly distributed and coordinated with the sulfur atoms in the DUT-67 ligands. This modification not only elevates the oxygen vacancy content but also broadens the light response range. A Schottky barrier is established at the Ag-DUT-67 interface, which effectively reduces carrier recombination. Notably, Ag-DUT-67–2 demonstrates a remarkable Cr(VI) reduction efficiency of 98% within 30 min, with a reaction rate that is 3.4 times as much as pristine DUT-67. Additionally, Ag-DUT-67–2 shows excellent stability in high-concentration Cr(VI) solutions and in the presence of interfering ions, coupled with good recyclability. This study offers a novel framework of interface engineering and performance enhancement of MOF-based photocatalysts for heavy metal reduction.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Yulong Xiang,Xinbin Ji,Xiaoli Dong,Yu Wang,Nan Zheng,Jialin Niu,Pei Yu,Chumin Yan
As Cr(VI) pollution intensifies, the development of efficient, eco-friendly, and sustainable treatment technologies has become a vital focus in environmental science. Photocatalytic reduction is often seen as a promising approach for removing Cr(VI), thanks to its low energy requirements and minimal environmental impact. However, traditional photocatalytic materials face significant challenges, including narrow photoresponse range and high rate of electron-hole recombination, which impede their practical efficiency. In this study, we successfully synthesized Fe-DUT-67 photocatalysts by incorporating Fe single atoms into the zirconium-based metal–organic framework (DUT-67) through post-synthetic modification. A significant enhancement in both the visible-light absorption capacity and carrier separation efficiency of the as-prepared Fe-DUT-67 has been observed, attributed to the formation of Fe-O coordination bonds between the Fe atoms and Zr-O clusters. Fe-DUT-67-2 exhibited impressive Cr(VI) reduction activity under full-spectrum illumination, with a remarkable 90% reduction efficiency of Cr(VI) within 18 min. Density functional theory (DFT) calculations shed light on the crucial role of Fe sites in promoting photoelectron transport and facilitating Cr(VI) reduction. This work not only presents an efficient photocatalytic material for alleviating Cr(VI) pollution but also provides a theoretical foundation and design principles for the development of high-performance catalytic systems utilizing single-atom modified metal–organic frameworks.
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2019
·Vol. 149
·期 7
·1845-1855
·
IF 2.372
Wang Tao,Hu Aiyun,Xu Guangzhi,Liu Chen,Wang Haijun,Xia Yongmei
Furfural (FAL) is one of the most important biomass-derived platform compounds. The catalytic transformation of FAL was investigated with three porous Zr–thiophenedicarboxylate hybrids for the production of furfuryl alcohol (FOL). Three Zr-based catalysts, including DUT-67(Zr), DUT-68(Zr) and DUT-69(Zr) were synthesized through a facile assembly of 2,5-thiophenedicarboxylate acid with ZrCl 4 using the acetic acid as a modulator under hydrothermal conditions. These catalysts were also characterized using FT-IR, XRD, SEM, TEM, N 2 adsorption–desorption, XPS and TG. The specific surface area of the DUT-69(Zr) is smaller than that of the DUT-68(Zr) and slightly larger than that of the DUT-67(Zr), but it has a relatively large pore volume and pore diameter. Although all three catalysts showed excellent catalytic activity towards the catalytic transfer hydrogenation of FAL into FOL, the DUT-69(Zr) material has slightly higher catalytic activity than the other two catalysts. Besides, considering the cost of catalyst preparation, the DUT-69(Zr) material was used as the optimal catalyst and studied in detail. A high FOL yield of 92.2% at 95.9% FAL conversion was achieved at 120 °C for 4 h over DUT-69(Zr). Meanwhile, the DUT-69(Zr) could be reused more than six times with a minor decrease in catalytic activity. Finally, a plausible mechanism for catalytic transfer hydrogenation of carbonyl compounds to produce corresponding alcohols was presented based on the results of the experiments and previous reports. Graphical Abstract
研究领域:
化学
·
材料科学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yiyang Bi,Kun Xu,Ying Wang,Xin Li,Xupeng Zhang,Jiabo Wang,Yu Zhang,Qun Liu,Qianrong Fang
Metal-organic framework materials (MOFs) and their derivatives have been widely used in the field of photocatalytic water decomposition for hydrogen production . In this study, NiS/CdS was initially acquired and subsequently combined with DUT-67 via ultrasound to create a unique ternary photocatalyst NiS/CdS@DUT-67. The rate of hydrogen production for NiS/CdS@DUT-67 is 9618 μmol·g NiS/CdS −1 ·h −1 for NiS/CdS@DUT-67, which is 32 times and 2.5 times higher than that for CdS and NiS/CdS, respectively. Of particular interest is the fact that even after 50 h of photocatalysis, the hydrogen production rate did not show a significant decrease, demonstrating its excellent stability compared to CdS and NiS/CdS. In this ternary system, NiS and DUT-67 function as dual co-catalysts for CdS, collaborating to enhance charge separation during the photocatalysis. This study presents a clear demonstration of the advantages of utilizing metal–organic framework derivatives (MOF-derivatives) cophotocatalysts and their synergistic effect, resulting in improved photocatalytic activity and stability of semiconductors. This innovative approach provides a new perspective on constructing photocatalytic materials with exceptional performance.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子