JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Longting Qi,Yujing Xie,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Bi 2 MoO 6 has drawn considerable attention in the field of photocatalysis owing to its excellent visible light response and photo-generated carriers transport ability. However, pure Bi 2 MoO 6 suffers from the limited surface-active sites and poor photogenerated charge separation efficiency, resulting in unsatisfactory photocatalytic performance. Herein, the 2D/2D Bi 2 MoO 6 /BiOBr Z-scheme heterojunction photocatalysts were synthesized by in-situ hydrothermal growth of Bi 2 MoO 6 on BiOBr. The optimized heterojunction catalyst, Bi 2 MoO 6 /BiOBr-40 % exhibited a CH 3 OH yield of 6.21 μmol·g -1 ·h -1 , which was twice that of the pure Bi 2 MoO 6 . Simultaneously, mechanism study by the band potential estimation and electron spin resonance (ESR) analysis evidenced that the enhanced activity was ascribed to the Z-scheme. This unique structure could enhance the spatial separation of electron-hole pairs, remain the strong redox ability. Moreover, the density functional theory (DFT) calculations were carried out to further expose the charge transfer mechanism of composites. This paper provided a novel approach for the design and manufacture of 2D/2D Z-scheme heterojunctions for energy conversion and environmental remediation.
研究领域:
材料科学
·
环境科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2025
·
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
·
材料科学
·
环境化学
·
化学工程
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Lijun Xue,Jie Zhang,Chenhui Qiu,Hui Wan,Guofeng Guan
The incorporation of Cu-species, leveraging their variable valence states, represents a promising strategy for enhancing photocatalytic CO2 reduction. However, the underlying mechanism through which multivalent Cu-species facilitate this process remains inadequately elucidated, motivating further investigation. Herein, multivalent copper-modified SrTiO3 nanofibers (CuxO/STO-Y) were synthesized via an electrospinning method combined with a glucose-assisted hydrothermal process. The optimized CuxO/STO-2 nanofiber photocatalyst demonstrated a CO2 photoreduction rate to CH3OH of 7.26 μmol g−1 h−1. According to the characterization results, loading CuxO species onto the SrTiO3 nanofiber surface can broaden the light-responsive range, further improving the separation efficiency of electrons and holes. The density functional theory (DFT) calculations revealed that photogenerated electrons from SrTiO3 preferentially migrated and accumulated on CuxO sites, thereby prolonging charge carrier lifetimes and ultimately improving the CO2 photoreduction efficiency. This work highlights the crucial role of valent-engineered Cu-species in enhancing the performance of photocatalysts.
研究领域:
光催化
·
材料科学
·
环境化学
·
能量转换
·
纳米材料
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Xiaoli Yang,Hongmin Duan,Ruifeng Wang,Fengwang Zhao,Fayi Jin,Wei Jiang,Guangting Han,Qingxin Guan,Haoxi Ben
The utilization of Cu-based catalysts in CO2 conversion into valuable chemicals is of significant interest due to their potential in mitigating greenhouse gas emissions. However, the controllable design of Cu-based catalysts and the regulation of their mechanism remain challenging. In this study, a series of efficient Cu/L catalysts were prepared for this process, and the intrinsic influencing factors on the reaction routes were systematically revealed. Various techniques revealed that Cu particles in L-supported catalysts exhibited higher dispersion and formed Cu–O(OH)–K interfacial sites. However, with increasing Cu loading, the dispersion of Cu particles and the percentage of Cu–O(OH)–K interfaces decreased. Kinetic investigations revealed that the adsorption configuration and electronic structure of Cu species codetermined the reaction pathways and resulting selectivity. Cu/L catalysts possessing Cu–O(OH)–K interfaces and small particles demonstrated the preferential formation of formate species, promoting methanol formation. However, larger Cu particles generated carboxylate intermediates, resulting in higher CO selectivity..
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2012
·
IF 0.826
Huiling CHEN,Shuanjin WANG,Min XIAO,Dongmei HAN,Yixin LU,Yuezhong MENG
The 0.4 nm molecular sieve supported Cu-Ni bimetal catalysts for direct synthesis of dimethyl carbonate (DMC) from CO 2 and CH 3 OH were prepared and investigated. The synthesized catalysts were fully characterized by BET, XRD (X-ray diffraction), TPR (temperature programmed reduction), IR (infra-red adsorption), NH 3 -TPD (temperature programmed desorption) and CO 2 -TPD (temperature programmed desorption) techniques. The results showed that the surface area of catalysts decreased with increasing metal content, and the metals as well as Cu-Ni alloy co-existed on the reduced catalyst surface. There existed interaction between metal and carrier, and moreover, metal particles affected obviously the acidity and basicity of carrier. The large amount of basic sites facilitated the activation of methanol to methoxyl species and their subsequent reaction with activated carbon dioxide. The catalysts were evaluated in a continuous tubular fixed-bed micro-gaseous reactor and the catalyst with bimetal loading of 20% (by mass) had best catalytic activities. Under the conditions of 393 K, 1.1 MPa, 5 h and gas space velocity of 510 h −1 , the selectivity and yield of DMC were higher than 86.0 % and 5.0 %, respectively.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Chenhui Qiu,Lei Wang,Ruijie Chen,Jie Zhang,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Perovskite-type LaFeO3 is regarded as a potentially efficient visible-light photocatalyst owing to its narrow bandgap energy and unique photovoltaic properties. However, the insufficient active sites and the unsatisfactory utilization of photogenerated carriers severely restrict the realistic application of pure LaFeO3. Herein, we fabricated a series of LaxFeO3−δ nanofibers (x = 1.0, 0.95, 0.9, 0.85, 0.8) with an A-site defect via sol–gel combined with the electrospinning technique. Wherein, the nonstoichiometric La0.9FeO3−δ possessed the highest CH3OH yield of 5.30 μmol·g–1·h–1 with good chemical stability. A series of advanced characterizations were applied to investigate the physicochemical properties and charge-carrier behaviors of the samples. The results illustrated that the one-dimensional (1D) nanostructures combined with the appropriate concentration of vacancy defects on the surface contributed to the radial migration of photogenerated carriers, inhibited the recombination of carriers, and provided more CO2 adsorption-activation sites. Furthermore, density functional theory (DFT) calculations were employed to reveal the influence mechanism of vacancy defects on LaFeO3. This work provides a strategy to enhance the performance of photocatalytic CO2 reduction by modulating the induced oxygen vacancies caused by the A-site defect in perovskite oxides.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jia-Yi Shi,Zhen-Long Wang,Ke-An Wang,Hai-Bin Zhu
The electrochemical reduction of carbon dioxide into energy-carrying compounds or value-added chemicals is of great significance for diminishing the greenhouse effect. However, it is still imperative to replace the less-value anodic oxygen evolution reaction (OER) to improve the technical economy. Herein, we firstly reported a bifunctional CuS/TiO 2 catalyst for both anodic methanol oxidation reaction (MOR) and cathodic carbon dioxide reduction (CO 2 R). The in-built abundant CuS/TiO 2 heterointerfaces are found to boost the CO 2 R and MOR to produce formate. Based on the unique bifunctionality of CuS/TiO 2 , a paired electrosynthesis of formate was performed with a total Faradaic efficiency (FE) of about 170 %, in which the cathodic CO 2 R achieved a formate FE of about 70 %, and the anodic MOR exhibited an almost 100 % formate FE.
研究领域:
化学
·
能源科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Hu Changjiang,Jiang Zhiwen,Wu Qunyan,Cao Shuiyan,Li Qiuhao,Chen Chong,Yuan Liyong,Wang Yunlong,Yang Wenyun,Yang Jinbo,Peng Jing,Shi Weiqun,Zhai Maolin,Mostafavi Mehran,Ma Jun
The efficient use of renewable X/γ-rays or accelerated electrons for chemical transformation of CO 2 and water to fuels holds promise for a carbon-neutral economy; however, such processes are challenging to implement and require the assistance of catalysts capable of sensitizing secondary electron scattering and providing active metal sites to bind intermediates. Here we show atomic Cu-Ni dual-metal sites embedded in a metal-organic framework enable efficient and selective CH 3 OH production (~98%) over multiple irradiated cycles. The usage of practical electron-beam irradiation (200 keV; 40 kGy min −1 ) with a cost-effective hydroxyl radical scavenger promotes CH 3 OH production rate to 0.27 mmol g −1 min −1 . Moreover, time-resolved experiments with calculations reveal the direct generation of CO 2 •‒ radical anions via aqueous electrons attachment occurred on nanosecond timescale, and cascade hydrogenation steps. Our study highlights a radiolytic route to produce CH 3 OH with CO 2 feedstock and introduces a desirable atomic structure to improve performance.
研究领域:
化学
·
材料科学
·
环境科学
·
辐射化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Yuxuan Wang,Chenhui Qiu,Yujing Xie,Lei Wang,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Using perovskite photocatalytic reduction of CO2 and H2O to produce hydrocarbon fuels offers an attractive method to solve the energy crisis and the greenhouse effect. Bi4Ti3O12 (BTO) has received much attention in the field of photocatalysis due to its unique layered structure, but it still faces many challenges such as weak photoresponse and severe photogenerated carrier recombination. In this paper, Bi4Ti3O12 nanosheets with different concentrations of surface oxygen vacancies (VO) and Ti3+ defect were prepared by the molten salt method and NaBH4 high-temperature reduction method (HBTO). Surface defects formed obvious carrier traps on the HBTO surface, reduced the recombination rate of photogenerated electrons and holes, and adjusted the band gap structure (from 3.09 to 2.62 eV), which improved the visible light utilization of HBTO. The decrease of photoinduced carrier recombination rate and the improvement of visible light response significantly enhanced the photocatalytic CO2 reduction activity of HBTO under visible light. The CH3OH yield with the optimized HBTO-4 (NaBH4:Bi4Ti3O12 = 1:5) was 4.90 μmol·g–1·h–1, which was about 3.5 times that of the original BTO. Meanwhile, the band gap structure, electronic density of states (DOS), and work function were calculated by the density functional theory (DFT). This study provided an effective strategy for designing and preparing perovskite photocatalysts rich in surface defects for the efficient conversion of solar energy.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Qin Jiao,Binchuan Gao,Li Zhang,Ruijie Chen,Lei Wang,Qiang Wang,Nengjie Feng,Hui Wan,Guofeng Guan,Mingjuan Han
The photocatalytic performance of graphitic carbon nitride (g-C 3 N 4 ) in the conversion of CO 2 to CH 3 OH is intrinsically constrained by its limited selectivity and activity. Herein, we developed a dual-modification strategy that integrates S doping into the g-C 3 N 4 (CN) skeleton and constructed a 2D/2D S-doped g-C 3 N 4 /Bi 2 MoO 6 Z-scheme heterojunction (SCN/BMO) via microwave-assisted synthesis. This strategy achieved sulfur doping through N-site substitution to modulate the electronic structure of CN, resulting in the formation of a 2D/2D SCN/BMO Z-scheme heterojunction. The optimized 0.3SCN/BMO photocatalyst achieved a methanol production rate of 6.19 μmol·g −1 ·h −1 with 99.15 % selectivity under solar irradiation, showing a 5.16-fold and 2.60-fold enhancement in catalytic activity compared to pristine g-C 3 N 4 and Bi 2 MoO 6 (BMO), respectively. Meanwhile, it demonstrated excellent photocatalytic and structural stability during the cycling tests. Systematic characterization analyses have revealed that the synergistic light-harvesting effect, optimized interfacial coupling, and efficient charge transport pathways within the 2D/2D 0.3SCN/BMO Z-scheme heterostructure collectively contribute to the significant enhancement in photocatalytic performance. Moreover, a feasible photocatalytic mechanism has been put forward by combining the outcomes of in-situ DRIFT spectroscopic analysis with DFT computational modeling. This research finding provides an innovative strategy for the development of highly efficient photocatalysts, which are specifically designed for the selective reduction conversion of CO 2 to CH 3 OH.
研究领域:
材料科学
·
环境科学
·
催化
·
纳米技术
·
物理化学
·
能量转换
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Weijia Li,Lingchu Huang,Tong Wang,Xidong Hao,Bin Wang,Qi Lu,Xishuang Liang,Fengmin Liu,Fangmeng Liu,Chenguang Wang,Geyu Lu
The development of high-performance gas sensors for detecting trace amount of CH 3 OH is an essential and a challenging task for safety using fuel cell vehicles (FCVs). In this work, the metal oxides (SnO 2 , In 2 O 3 , CuO) are employed as the catalyst carrier materials in fuel cell type sensors for the first time to replace traditional carbon, with which the Pt/MO x based fuel cell type sensors are fabricated. Among them, Pt/SnO 2 based sensor displays the lowest detection limit because SnO 2 carrier can not only support Pt particles but also provide an appropriate number of electrons for Pt, which is beneficial to reduce the adsorption strength of the intermediates and then improves the catalytic ability. The detection limit is as low as 0.5 ppm, the lowest of the various types of CH 3 OH sensors that work at room temperature. Moreover, the Pt/SnO 2 based fuel cell type sensor displays the characters of high selectivity, good repeatability and robust moisture resistance. To the best of our knowledge, this is the first report employing MO x as the catalyst carrier materials in fuel cell type sensors.
研究领域:
材料科学
·
传感器技术
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Xiushuai Guan,Shanbiao Jin,Le Liu,Xiya Zhao,Xiaochao Zhang,Changming Zhang,Zhong Li,Caimei Fan
The utilization of oxygen vacancies to modulate the surface properties of catalysts is a powerful way to enhance catalytic activity. In this work, the doping effect of Bi 3+ on the performance of CeO 2−δ (Ce x Bi 1−x O 2−δ ) hybrid nanorods with rich oxygen vacancies for the photo-thermal synthesis of dimethyl carbonate (DMC) from CO 2 /CH 3 OH (140 ℃, 1.6 MPa, 4 h) is systematically investigated. It is found that Ce 0.9 Bi 0.1 O 2−δ exhibits the best catalytic performance, achieving a photo-thermal yield of 3.13 mmol∙g −1 without any dehydrating agent (1.14 times compared to thermal catalysis). It turns out that regulating the concentration of Bi 3+ ions not only modifies the oxygen vacancy content, but also improves the light harvesting efficiency. Moreover, a series of characterization techniques, such as X-ray photoelectron spectroscopy, Raman spectrometer and electron paramagnetic resonance are employed to analyze and verify that the asymmetric oxygen vacancies are conducive to the improvement in the CO 2 adsorption-activation. Finally, a possible reaction mechanism model of Bi 3+ doping on CeO 2−δ for the photo-thermal synthesis of DMC from CO 2 and CH 3 OH is proposed. This work provides a practical approach to catalyst surface engineering design.
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 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）