ADVANCED MATERIALS
·
2019
·Vol. 31
·期 36
·1903499
·
IF 25.809
Shiyong Mou,Tongwei Wu,Junfeng Xie,Ya Zhang,Lei Ji,Hong Huang,Ting Wang,Yonglan Luo,Xiaoli Xiong,Bo Tang,Xuping Sun
Electrocatalysis has emerged as an attractive way for artificial CO 2 fixation to CH 3 OH, but the design and development of metal-free electrocatalyst for highly selective CH 3 OH formation still remains a key challenge. Here, it is demonstrated that boron phosphide nanoparticles perform highly efficiently as a nonmetal electrocatalyst toward electrochemical reduction of CO 2 to CH 3 OH with high selectivity. In 0.1 m KHCO 3 , this catalyst achieves a high Faradaic efficiency of 92.0% for CH 3 OH at −0.5 V versus reversible hydrogen electrode. Density functional theory calculations reveal that B and P synergistically promote the binding and activation of CO 2 , and the rate-determining step for the CO 2 reduction reaction is dominated by *CO + *OH to *CO + *H 2 O process with free energy change of 1.36 eV. In addition, CO and CH 2 O products are difficultly generated on BP (111) surface, which is responsible for the high activity and selectivity of the CO 2 -to-CH 3 OH conversion process.
研究领域:
电催化
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材料科学
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可持续能源
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二氧化碳利用
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纳米催化剂
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Xiangqian Guo,Chenhui Qiu,Zhiqiang Zhang,Jie Zhang,Lei Wang,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic CO 2 reduction plays an important role in solving environmental issues and alleviating the energy crisis. However, it is still challenging to distribute the surface-active site on photocatalysts with efficient separation of carriers in rational. Herein, the Cu species loaded SrTiO 3 nanofiber was constructed through coaxial electrospinning which could realize the dispersion of the Cu site on the one-dimensional (1D) nanofiber structure. The 1D nanofiber with Cu site exhibited superior performance on photocatalytic CO 2 reduction based on the excellent ability of charge separation. The Cu 2 O and CuO were determined to be located on the surface of 1D SrTiO 3 nanofiber by the TEM and XPS. The work functions of SrTiO 3 , Cu 2 O, and CuO were calculated to be 5.26, 5.47, and 5.51 eV, respectively, suggesting that the carriers could transfer from SrTiO 3 nanofiber to the Cu species. The yield of CH 3 OH with the optimized 8%Cu-SrTiO 3 catalyst could reach 8.08 ± 0.03 µmol⋅g −1 ⋅h −1 . This work provided a coaxial electrospinning strategy to load the Cu species active site on the surface of 1D SrTiO 3 nanofiber for enhancing photoreduction CO 2 .
研究领域:
材料科学
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环境科学
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能源科学
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纳米技术
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产品关联
DOI
高影响因子
Nature Catalysis
·
2022
·Vol. 5
·期 1
·45-54
·
IF 40.706
Qi Guodong,Davies Thomas E.,Nasrallah Ali,Sainna Mala A.,Howe Alexander G. R.,Lewis Richard J.,Quesne Matthew,Catlow C. Richard A.,Willock David J.,He Qian,Bethell Donald,Howard Mark J.,Murrer Barry A.,Harrison Brian,Kiely Christopher J.,Zhao Xingling,Deng Feng,Xu Jun,Hutchings Graham J.
The oxidation of methane, the main component of natural gas, to selectively form oxygenated chemical feedstocks using molecular oxygen has been a long-standing grand challenge in catalysis. Here, using gold nanoparticles supported on the zeolite ZSM-5, we introduce a method to oxidize methane to methanol and acetic acid in water at temperatures between 120 and 240 °C using molecular oxygen in the absence of any added coreductant. Electron microscopy reveals that the catalyst does not contain gold atoms or clusters, but rather gold nanoparticles are the active component, while a mechanism involving surface adsorbed species is proposed in which methanol and acetic acid are formed via parallel pathways.
研究领域:
催化化学
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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
Molecular Catalysis
·
2026
·
IF 4.3
Song Wu,Xiangqian Guo,Chenhui Qiu,Jinfeng Zhang,Hui Wan,Guofeng Guan
Light-driven CO 2 conversion to high-value chemicals has emerged as promising but challenging strategy to alleviate global energy and environmental concerns. The efficacy of this process hinges critically on the design of advanced catalysts. Herein, the metallic co-catalysts Pt deliberately anchored onto the surface of La 0.8 Sr 0.2 Co 0.7 Fe 0.3 O 3 (LSCFO) nanotubes was constructed via direct coaxial electrospinning method. Experimental analyses and density functional theory (DFT) simulations confirmed that the incorporation of Pt creates additional active sites and suppresses the recombination of photo-generated electron-hole pairs, thereby enhancing photocatalytic CO 2 reduction capability. Under visible light illumination, the optimized Pt 6 /LSCFO catalyst demonstrated a remarkable CH 3 OH yield of 7.20 μmol·g⁻¹·h⁻¹, outperforming pristine LaCoO 3 by a factor of 3.48. Moreover, the catalyst retains its structural integrity and catalytic performance over four consecutive cycles, demonstrating excellent stability. This work presents an integrated strategy via one-step coaxial electrospinning method for constructing high-performance composite photocatalysts.
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 2
·121314
·
IF 7.2
Gangye Cen,Weiqun Chu,Jianfeng Lu,Jing Ding,Yukun Hu,Weilong Wang
Photocatalytic reduction of CO 2 to methanol using water as a proton source offers a sustainable pathway for solar energy storage and carbon neutrality. However, its practical application is hindered by low quantum efficiency, rapid charge recombination, and reliance on sacrificial agents. Herein, we developed a bimetallic AuCu alloy supported on TiO 2 nanoparticles (AuCu-TiO 2 ) via a NaBH 4 reduction method for efficient CO 2 -to-methanol conversion in the absence of sacrificial agents. The photocatalytic performance was correlated with in situ FTIR spectroscopy to unravel the synergistic roles of AuCu alloy sites and TiO 2 in mediating CO 2 reduction and H 2 O oxidation. CO 2 activation by photogenerated electrons leads to the formation of critical intermediates like COOH* and CHO*, which undergo sequential hydrogenation to produce methanol. The Au-Cu synergy facilitates the hydrogenation of COOH* to CHO*, significantly boosting methanol selectivity. By optimizing the AuCu loading and Cu/Au molar ratio, the AuCu-TiO 2 catalyst achieved a high methanol production rate of 63.31 μmol g −1 h −1 with 85.59 % selectivity. This work provides a general strategy for designing efficient bimetallic photocatalysts for selective CO 2 conversion under environmentally benign conditions.
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DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 9
·889
·
IF 4
Lijun Xue,Yuxuan Wang,Chenhui Qiu,Hui Wan
Developing highly efficient photocatalysts for CO2reduction remains a great challenge. The large band gap and poor charge carrier dynamics are the major factors limiting the performance of Bi4Ti3O12(BTO). Herein, a series of La-doped Bi4Ti3O12(BLaxTO) nanosheets were synthesized and further modified by NaBH4hydrogenation to create surface defect-rich H-BLaXTO nanosheets. Characterizations and theoretical calculations confirmed that the synergistic effect of La doping and hydrogenation significantly enhanced visible-light absorption, promoted charge separation, and improved the electron reduction capacity. When applied to photocatalytic CO2reduction, the H-BLa0.2TO catalyst achieved a superior CH3OH production rate of 7.90 μmol·g−1·h−1, which is 5.6 times higher than that of pristine Bi4Ti3O12. Moreover, the H-BLa0.2TO catalyst maintained excellent stability over four consecutive cycles. This study offers an integrated strategy for constructing high-performance bismuth-based photocatalysts through elemental doping and defect engineering.
研究领域:
材料科学
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光催化
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环境化学
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能源化学
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纳米材料
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表面科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Chenhui Qiu,Lei Wang,Ruijie Chen,Gongde Wu,Jie Zhang,Jing Ding,Jun Li,Jinfeng Zhang,Hui Wan,Guofeng Guan
Synthesizing value-added solar fuels represents a promising solution to address energy and environmental issues. Its efficiency is determined by the performance of photocatalysts, and the main challenges lie in achieving efficient interfacial charge transfer and utilization, which are highly related to the assembly of cocatalysts. Herein, we design La 3+ -defect LaFeO 3 nanofibers with a higher specific surface area to achieve highly dispersed loading of Ag nanoparticles through a one-step coaxial electrospinning technique. Characterizations and theoretical calculations revealed that La 3+ defects favor the anchoring of Ag nanoparticles and the formation of a Schottky junction, thereby facilitating the interfacial charge separation and transfer. Additionally, this synergistic engineering efficiently boosts CO 2 adsorption/activation and strengthens the proton affinity, preferentially driving the multi-electron reduction. Owing to these benefits, the optimized nanofibrous Ag/La 0.9 FeO 3 sample exhibits promising photothermal catalytic performance, yielding CH 3 OH of 7.12 μmol·g -1 ·h -1 , which is 2.8-fold over pristine LaFeO 3 , along with good stability and selectivity. This work highlights the effect of interfacial construction on developing advanced photocatalysts.
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产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Yujing Xie,Chenhui Qiu,Lei Wang,Yuxuan Wang,Jie Zhang,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic CO 2 reduction to fuels via visible light is regarded as a highly promising sustainable technology to address resource depletion and environmental apprehensions. However, the elevation of photocatalytic performance is limited due to some drawbacks of isolated catalysts such as poor CO 2 adsorption performance, inadequate utilization of visible light, and rapid recombination of photo-generated carriers. Herein, a series of novel heterojunction catalysts, 1D/2D CeO 2 /Bi 2 MoO 6 (CBMO-X), were fabricated utilizing the microwave-assisted method for the photocatalytic reduction of CO 2 . The CH 3 OH yield of the optimized CBMO-10 composite material reached 4.31 μmol⋅g −1 ⋅h −1 with excellent stability and structural integrity. Through a series of characterizations, it was found that the introduced CeO 2 nanorods served as bifunctional sites for CO 2 adsorption and photoelectron accumulation, effectively promoting CO 2 conversion under visible light. In addition, CBMO-X exhibited faster photo-generated carriers migration rate due to the formation of the II-scheme heterojunction, which improved the photocatalytic performance obviously. Furthermore, the density functional theory (DFT) calculations and in situ XPS were used to investigate the carrier migration paths on the surface of composite materials. This work provided a novel strategy for the design of photocatalysts for efficient CO 2 conversion.
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Hailong Tang,Yongqing Ma,Ganhong Zheng,Chuhong Zhu,Meiling Wang,Yilin Lu,Xiao Sun
Photocatalytic CH 4 conversion to CH 3 OH under mild conditions is undoubtedly an efficient strategy to realize CH 4 upgrading. In this work, in-situ formed highly reactive Fe IV =O complex with a bound Cl axial ligand was detected at ambient temperature and its contribution to CH 4 photoxidation to CH 3 OH was deeply investigated. Under optimized experimental condition, a high CH 3 OH yield of 3026.1 mmol mol Fe −1 (6.76 mmol g cat −1 h −1 ) with selectivity of 73.6 % was obtained during 8 h. Isotope labeling mass spectroscopy experiments manifested that O 2 was the only source of oxygen in products. The formation of Cl-(H 2 O) 4 Fe IV O complex was confirmed using low-temperature electron spin resonance spectroscopy and cryogenic Raman spectroscopy (ν(Fe O) = 828 cm −1 ). Through density functional theory (DFT) calculation, we showed that the Cl axial ligand acts as an “electron reservoir” during CH 4 conversion, i.e., electron acceptor during the process of CH 4 oxidation to CH 3 OH, while electron donor in CH 3 OH desorption. This not only lowered C-H cleavage energy, but also facilitated CH 3 OH desoption and inhibited overoxidation. As far as we know, Cl-(H 2 O) 4 Fe IV O is the first detected Fe IV O complex generated directly from O 2 and Fe 3+ at ambient temperature.
研究领域:
化学
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环境科学
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产品关联
DOI
高影响因子
ACS Omega
·
2026
·
IF 5.2
Malesela A. Mafokoane,Peixi Liu,Xiaoxia Ou,Nicholas M. Musyoka,Fei Chang
The reduction of carbon dioxide (CO2) to methanol (CH3OH), is presently constrained by energy-intensive processes requiring high temperatures and pressures to overcome kinetic and thermodynamic limitations. This work unveils for the first time a reaction pathway for alkali and alkaline earth metal hydrides (LiH, NaH, KH, MgH2, CaH2, and BaH2), enabling the activation and selective reduction of CO2 to methanol under ambient pressure. This finding represents a significant departure from the established paradigm, which exclusively produced methane at moderate pressures (0.1–1 MPa). Temperature-programmed reaction studies reveal that these metal hydrides function synergistically as both hydrogen sources and promoters for CO2 reduction, exhibiting hydrocarbon production within specific temperature windows. Systematic screening identifies lithium hydride (LiH) as the most effective material, with a maximum production rate of 0.182 μmolMeOH·molmetal–1·h–1 at 245 °C under ambient pressure, highlighting a structure–activity relationship governed by metal-formate stability. Through mechanistic investigation, we elucidate a formate (HCOO*)-mediated pathway wherein the hydride ion serves as a potent nucleophile, directly reducing CO2 without the need for high H2 partial pressures. This discovery provides a transformative framework for the sustainable synthesis of CH3OH and lays the groundwork for the development of next-generation materials incorporating reactive ionic hydrides for the conversion of CO2 under mild conditions.
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Bingke Yang,Haojie Li,Zhen Yao,Lili Xing,Xuetao Wang,Yilin Zhu
In the study, ammonia borane alcoholysis with different types of alcohols (CH3OH, CH3CH2OH, (CH2OH)2) for hydrogen production are investigated, and the effects of different pressures and temperatures on the adsorption properties are also investigated using the DFT calculation and experimental method. In the ammonia borane alcoholysis, NH3BH3 molecules and alcohols molecules (R-OH) are first adsorbed onto the active metal surface, where the hydroxyl groups in the R-OH molecules are activated and the O-H bonds are broken to produce the intermediates H* and *O-R. Further a strong interaction between the B in NH3BH3 and the O in *O-R occurs and the B-N bond is broken, forming the intermediate products *NH3, *BH2-O-R and another H*, H2 molecule is released during B-O bonding with one of the H originated from the hydroxyl group and the other originated from the *HB in the NH3BH3 molecule. The energy barriers for the ammonia borane alcoholysis with CH3OH, CH3CH2OH and (CH₂OH)₂ are 28.23 kcal/mol, 37.5 kcal/mol and 42.32 kcal/mol, respectively, which results in a different alcoholysis rate of ammonia borane AB/CH3OH> AB/CH3CH2OH> AB/(CH2OH)2 at the macroscopic level. The high pressure enhances the adsorption properties of ammonia borane and alcohol molecules, while the high temperature decreases the adsorption properties. The adsorption capacities of ammonia borane and alcohols on the active metal Ru (101) are CH3OH (0.32 mmol/g) < NH3BH3 (1.03 mmol/g) < CH3CH2OH (1.05 mmol/g) < (CH2OH)2 (1.31 mmol/g) specifically. The results of this study provide a theoretical basis for the regulation of hydrogen production from ammonia borane alcoholysis.
研究领域:
化学工程
·
材料科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
Chem
·
2023
·
IF 23.5
Jie Ding,Zhenyuan Teng,Xiaozhi Su,Kosaku Kato,Yuhang Liu,Ting Xiao,Wei Liu,Lingyue Liu,Qiao Zhang,Xinyi Ren,Jincheng Zhang,Zhaoyang Chen,Ohno Teruhisa,Akira Yamakata,Hongbin Yang,Yanqiang Huang,Bin Liu,Yueming Zhai
By breaking structural symmetry of the single atomic active site, the photocatalytic water oxidation pathway is tuned for highly selective oxidation of CH 4 to CH 3 OH in an aqueous solution. The water oxidation ability and its influence on photocatalytic oxidation of CH 4 over symmetrically coordinated cobalt single atom (Co-4N) on carbon nitride (SC-Co 1 /PCN) and asymmetrically coordinated cobalt single atom (Co-C2N2) on carbon nitride (AC-Co 1 /PCN KOH ) photocatalysts are systematically investigated. A super selectivity of 87.22% for photocatalytic oxidation of CH 4 to CH 3 OH is realized on AC-Co 1 /PCN KOH , which is only 45% on SC-Co 1 /PCN. Moreover, a CH 4 conversion of 2.42% and a CH 3 OH yield of 2.11% are achieved over AC-Co 1 /PCN KOH (200 mg). Combining multiple in-situ characterizations and time-dependent density functional theory calculations, it is revealed that AC-Co 1 /PCN KOH possesses a desired electronic configuration for single-electron transfer water oxidation reaction during photocatalysis, leading to a notably promoted selectivity for CH 4 oxidation to CH 3 OH under illumination.
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）