INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Qinxuan Cao,Jianning Feng,Jinzhong Zhang,Jie Xue,Kang Wang,Ye Yang,Haipeng Lu
Direct utilization of solar energy by semiconductor nanocrystals for chemical transformations via photocatalysis has recently drawn a great deal of attention. While most photocatalytic reactions are mediated through photoredox events, the ultimate reaction scalability relies on the use of sacrificial agents. The imbalanced population of photogenerated electrons and holes often leads to catalyst degradation through photocorrosion. To circumvent this, we designed Ni2+-doped CsPbBr3 nanoplatelets (NPls) as a “redox-neutral” photocatalyst, where both oxidative and reductive cycles occur in one photocatalyst. We showed that surface Ni2+ ions can act as an “electron shuttle” to reduce protons, generating clean-energy H2 gas, while the photogenerated holes can be used to oxidize diaryl hydrazines to afford valuable azobenzenes and derivatives. Compared with previous photocatalytic demonstrations, our catalysts show excellent reaction yields with a wide substrate scope, unity atomic efficiency, and enhanced stability and recyclability.
研究领域:
材料科学
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化学工程
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光化学
·
催化
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产品关联
DOI
PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Defu Yin,Renjie Ji,Jingyun Zhang,Shitao Yu,Lu Li,Shiwei Liu,Long Jiang,Ying Liu,Zhanqian Song,Yue Liu
A core–shell catalyst composed of mCeO 2 shell and Pd metal core was prepared by one-pot wet chemical method and used for the hydrogenation of phenol to cyclohexanone. The phenol conversion and cyclohexanone selectivity were 96.3 % and 95.3 % at reaction conditions of 50 min, 80 °C and 1 MPa H 2 . The effects of Ce species and Br species in the preparation of catalysts was studied, and the synthesis mechanism of core–shell Pd@mCeO 2 catalysts was preliminarily revealed. By discussing the phenol adsorption mechanism and the redox properties of the catalyst, the activation of H 2 by Pd sites and phenol by cerium oxide (CeO 2 ) sites of the surface were studied. H 2 -TPR and XPS characterization were used to explain the effect of Ce species and Br species for the catalytic performance. These results indicated that the electronic structure of Pd was regulated by the interaction between Pd and Ce, and different O sites were generated around the Pd sites. In situ IR spectra indicated that phenol was adsorbed and dissociated on cerium to form phenoxy species and water, this synergistic catalytic pattern of carrier activated substrate and hydrogenation site promoted the hydrogenation of phenol and improved the catalytic efficiency.
研究领域:
催化
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化学工程
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材料科学
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物理化学
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产品关联
DOI
高影响因子
Science Bulletin
·
2025
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IF 21.1
Tongtong Yang,Heng Liu,Hengjie Liu,Weiyi Zhao,Jiawei Ge,Wenhui Wang,Shuai Yang,Meijian Tang,Kai Wei,Kangcheng Wang,Zeming Qi,Xian Wang,Hao Li,Junjie Ge
Single-atom catalysts (SACs) challenge conventional multi-site catalysis by enabling oxidative processes like H 2 and CO oxidation. However, we herein present that the completely isolated SACs are inactive, while spatially adjacent single-atom pairs (interatomic distance < 4 Å) work cooperatively as the true active sites. Rh atomic densities were precisely tuned between 0.1 wt%–17.5 wt% via graphene quantum dots confinement. Mathematical modeling quantifies the scaling of active pairs versus electrochemical performance, rationalizing activity dependence on atomic proximity. 18 O isotope labeling and in situ synchrotron infrared spectroscopy analyses identified a new reaction mechanism, with water bifunctional dissociation enabled on sub-4 Å Rh pairs, and acts as the rate-determining step towards both CO and H 2 oxidation. While H 2 O enters the COOR process as a reactant and enters the HOR process as a molecular catalyst. Our findings redefine bifunctional catalysis, merging single-atom precision with nanoparticle-like cooperativity for efficient energy conversion systems.
研究领域:
材料科学
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催化
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电化学
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能量转换
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2024
·Vol. 130
·期 10
·1-12
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IF 2.5
Tang Mingxin,Qin Cong,Sun Xueya,Li Mengwei,Wang Yihui,Cao Jianliang,Wang Yan
Hydrogen (H 2 ) energy, as a clean energy source, has high energy density and durability, while H 2 is flammable and explosive, which requires strict safety technology measures to ensure the safety of high-pressure storage transportation. Therefore, the development of sensitive sensors is needed. In this study, In 2 O 3 microspheres with different Pd loadings were fabricated by hydrothermal method. Compared with the pristine In 2 O 3 gas sensor, the optimal operating temperature of the In 2 O 3 sensor is reduced from 160 ℃ to 80 ℃ after loading Pd. Among the prepared Pd/In 2 O 3 gas sensors, the response value of the 2 at% Pd/In 2 O 3 sensor towards 1000 ppm H 2 is 50.743 at 80 ℃. The response/recovery time is 80 s/235 s. The improved H 2 sensing performance can be ascribed to the chemical and electron sensitization of Pd, and the formation of PdO, PdH x . This study shows that Pd-loaded In 2 O 3 can effectively reduce the optimal operating temperature and enhance the response value for detecting H 2 in the range of 5-5000 ppm. Therefore, this sensor has good application prospects for detecting H 2 at low temperatures.
研究领域:
材料科学
·
传感器技术
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产品关联
DOI
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2024
·
IF 4.1
Meng-Jie Cui,Shan-Shan Li,Tie-Zhen Ren,Abulikemu Abulizi,Ai-Sha Nulahong
H 2 evolution through photocatalysis possesses has the advantage for achieving the carbon neutral, that relies on the highly efficient catalysts. Non-noble metals have lower prices than noble metals, which is beneficial for their large-scale applications in industry. In this paper, functionalized CuNi alloy and BaTi 4 O 9 (BTO) composite (Cu x Ni y /BTO(Z)) photocatalyst were synthesized successfully through hydrothermal calcination method. The acetates were selected the raw material to avoid the use of hazardous chemicals and pollution of photocatalysts by other elements, while also providing C=O for the photocatalyst to further enhance its photocatalytic activity. Under visible light irradiation, the photocatalytic hydrogen (H 2 ) evolution rate of Cu 3 Ni/BTO is 184.14 μmol·g −1 ·h −1 , which is 101.18 times that of pure BTO (1.82 μmol·g −1 ·h −1 ) under the same conditions. Combining density functional theory (DFT) calculations and experimental studies, it is concluded that electronic structural characteristics of BaTi 4 O 9 and the addition of CuNi alloy could provide more electrons and improve the photocatalytic H 2 evolution activity.
研究领域:
材料科学
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能源科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Xiangjun Liu,Jingjing Ma,Shuai Zhang,Guo-Wei Guan,Qing-Yuan Yang,Junqi Wang
Harvesting solar energy to drive highly efficient photocatalytic conversion of renewable biomass to value-added chemicals and H 2, is a green and promising strategy to acquire clean H 2 with high energy density. In this study, CdS nanoparticles/Ti 3 C 2 T x nanosheets (Ti 3 C 2 T x /CdS composites) photocatalysts were prepared by a hydrothermal strategy. With an optimized Ti 3 C 2 T x loading of 0.8 wt%, the Ti 3 C 2 T x /CdS composites exhibited a significant enhancement in the photocatalytic H 2 evolution reaction with long-term stability, reaching 20,427 μmol·g −1 ·h −1 , compared to the pristine CdS (1,999 μmol·g −1 ·h −1 ). The Ti 3 C 2 T x /CdS-0.8 reflects appropriate electronic band structure and excellent conductivity, resulting in efficiently generation and migration of photoinduced electrons. In addition, the apparent quantum yield of Ti 3 C 2 T x /CdS-0.8 was 9.4% at 420 nm, higher than that of pristine CdS (1.2%). Superior results (7,164 μmol·h −1 ·g −1 ) were also achieved in the conversion of raw biomass to H 2 under natural sunlight. Achieving solar-driven H 2 production from biomass represents a significant step forward in contributing to sustainable and clean energy practices.
研究领域:
材料科学
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能源化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Changdie Cao,Yurun Dai,Zhihao Liu,Zong Lu,Mide Luo,Yanying Wei,Haihui Wang
Two-dimensional (2D) nanosheet membranes presented excellent gas separation performance, which has attracted increasing attention. The electrophoretic deposition (EPD) method provides a fast and scalable route for the preparation of 2D nanosheet membranes aimed at future industrial applications. However, the formation of bubbles via water electrolysis during EPD would damage the membrane structure, and the expansion of interlayer spacing would hinder its utilization. Herein, the solvent-mediated structural regulation strategy for MXene membrane preparation via EPD is proposed for H 2 purification. The effect of various organic solvents on the EPD-prepared MXene membrane structure and gas separation performance has been investigated. Notably, the MXene membranes deposited using acetone as solvent exhibit outstanding gas separation performance, boasting an H 2 /CO 2 selectivity of 374 with a H 2 permeance of 748 GPU for at least 450 h. This work offers a novel approach to fast fabricating 2D nanosheet membranes with outstanding gas separation performance
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
OPTICAL MATERIALS
·
2022
·
IF 3.754
Jian Lu,Hui Lin,Ruijin Hong,Dawei Zhang
By the solid phase reaction method, pure KNN and KNN with different proportions halloysite nanotubes (HNTs) were prepared to study the photocatalytic hydrogen evolution performance under the UV light irradiation. The band gaps of KNN with HNTs are narrower than that of pure KNN. The absorbance of KNN in the ultraviolet region is significantly enhanced by the incorporation of HNTs, where the absorbance in the 200-300 nm region increased about 2 times. Compared with KNN, the conduction band edge of KNN-5wt%HNTs reduced from −1.13 eV to −1.18 eV, showing stronger reducing ability. The H 2 production rate of KNN with HNTs is much higher than that of the raw KNN without HNTs. The best H 2 production rate of KNN-5wt%HNTs is 31.28 μmol•g −1 •h −1 , approximate 4.48 times as high as the rate of pure KNN (6.98 μmol•g −1 •h −1 ), suggesting appropriate addition of HNTs can efficiently improve the H 2 production efficiency.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2019
·
IF 12.221
Nengchao Luo,Tingting Hou,Shiyang Liu,Bin Zeng,Jianmin Lu,Jian Zhang,Hongji Li,Feng Wang
Photocatalytic H2 evolution from organic feedstocks with simultaneous utilization of photogenerated holes achieves solar energy storage and coproduces value-added chemicals. Here we show visible-light H2 production from benzyl alcohol (BAL) with controllable generation of deoxybenzoin (DOB) or benzoin (BZ) through tandem redox reactions. Particularly, DOB synthesis circumvents the use of expensive feedstocks and environmentally unfriendly catalysts that are required previously. Under the irradiation of blue LEDs, the key of steering the major product to DOB rather than BZ is to decrease the conduction band bottom potentials of the ZnIn sulfide catalysts by increasing the Zn/In ratio, which results in the dehydration of intermediate hydrobenzoin (HB) to DOB proceeding in a redox-neutral mechanism and consuming an electron–hole pair. As a proof of concept, this method is used to synthesize DOB derivatives in gram scale.
研究领域:
化学工程
·
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2016
·
IF 3.15
Bing Zhang,Yingxuan Li,Jianmin Luo,He Zhao,Jie Zhao,Guohui Dong,Yunqing Zhu,Chuanyi Wang
The SrBi 2 Nb 2 O 9 platelets with a thickness of about 600 nm were synthesized by molten salt synthesis method. The treatment of the SrBi 2 Nb 2 O 9 platelets with hydrochloric acid resulted in the formation of the protonated H 1.78 Sr 0.78 Bi 0.22 Nb 2 O 7 platelets. Through a top–down approach in ethylamine solution, the H 1.78 Sr 0.78 Bi 0.22 Nb 2 O 7 platelets were exfoliated into H 1.78 Sr 0.78 Bi 0.22 Nb 2 O 7 nanosheets with a thickness of about 2.6 nm. The evolution of the structure, composition, morphology, optical, and photocatalytic properties of SrBi 2 Nb 2 O 9 platelets was studied as it is converted into H 1.78 Sr 0.78 Bi 0.22 Nb 2 O 7 platelets and subsequently exfoliated into H 1.78 Sr 0.78 Bi 0.22 Nb 2 O 7 nanosheets. The absorption edge shifts to a lower wavelength accompanied by the protonation and exfoliation. The photocatalytic H 2 evolution of the three samples were evaluated under the irradiation of a 300 W Xenon lamp from CH 3 OH/H 2 O solution, indicating that H 1.78 Sr 0.78 Bi 0.22 Nb 2 O 7 nanosheets Exhibit 5.5 and 26.2 times higher activity than that of the H 1.78 Sr 0.78 Bi 0.22 Nb 2 O 7 and SrBi 2 Nb 2 O 9 platelets, respectively. The enhanced activity for the H 1.78 Sr 0.78 Bi 0.22 Nb 2 O 7 nanosheets is mainly attributed to the higher separation efficiency of the photogenerated carriers and the larger specific surface area caused by the significant reduction in thickness.
研究领域:
材料科学
·
能源科学
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2022
·
IF 10.319
Meng Dai,Zuoli He,Peng Zhang,Xin Li,Shuguang Wang
The recombination of photogenerated electrons and holes is a crucial factor limiting photocatalytic H 2 evolution. The S-scheme ZnWO 4 -ZnIn 2 S 4 heterojunction with 2D coupling interfaces was successfully synthesized using a simple solvothermal method. An effective S-scheme interfacial charge migration route at the S-scheme heterogeneous interface was determined by energy band structure analyses (such as UPS, Mott-Schottky and XPS plots), which facilitates the separation of photoexcited carriers. It is worth noting that the optimal ZnWO 4 -ZnIn 2 S 4 composite has an H 2 evolution activity of 4925.3 μmol g −1 h −1 with favourable photostability and stability. Meanwhile, the ZnWO 4 -ZnIn 2 S 4 heterojunction exhibits the maximum optical response value (2.8 mA cm −2 ) in the initial stage, effectively promoting the separation and migration of photogenerated carriers. The establishment of the built-in electric field direction at the interface can effectively promote the space charge separation between the ZnWO 4 and ZnIn 2 S 4 nanosheets, which is favorable to the photocatalytic H 2 evolution. This work provides valuable guidance for designing S-scheme heterojunction photocatalysts composed of two n-type semiconductors for energy and environmental applications.
研究领域:
材料科学
·
能源与环境科学
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS RESEARCH BULLETIN
·
2021
·
IF 4.641
Yao Chen,Xin Xin,Dong Yang,Hanjie Ren,Yuchen Gao,Zhanfeng Zhao,Wenjing Wang,Ke An,Jiangdan Tan,Zhongyi Jiang
Designing visible-light-driven, high-efficiency, robust photocatalysts with practical potential is an important direction in the photocatalysis field. Herein, pyrimidine-modified g-C 3 N 4 (Pym-CN) photocatalysts with curled nanosheet morphology were prepared through a facile supramolecular assembly method. Pyrimidine has only two N atoms, thus leading to the deficiency formation in the supramolecular assembly of cyanuric acid with melamine. Upon calcination, the deficiency decreases the polycondensation degree of g-C 3 N 4 , thereby further affecting its morphology and optoelectronic property. The pyrimidine modification can enhance the absorption capacity toward visible light and facilitates the separation of photo-generated carriers. By changing the adding amount of pyrimidine, the optimal Pym-CN photocatalyst exhibits a H 2 evolution rate of 1046 μmol g −1 h −1 under visible light, which is almost 30 times higher than that of pristine g-C 3 N 4 . This work may afford a novel approach to modifying organic polymer semiconductor photocatalysts with small organic molecules of nonplanar structure.
研究领域:
材料科学
·
光催化
·
纳米技术
·
化学
✓ 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）