APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Mazhar Khan,Zeeshan Akmal,Muhammad Tayyab,Seemal Mansoor,Dongni Liu,Ziwei Ye,Jinlong Zhang,Shiqun Wu,Lingzhi Wang
The rational design of heterojunction photocatalysts is crucial for enhancing CO 2 photoreduction efficiency, yet precisely channeling photogenerated electrons to the CO 2 adsorption sites remains an enormous challenge. In this work, we developed an organic-inorganic heterostructure with continuous inter- and intra-component electric fields. The integration of BiOBr with MIL-125 via chemical bonding established a heterojunction, where the built-in electric field between the two components facilitated the efficient transfer of photogenerated electrons from BiOBr to MIL-125. The intrinsic electric field of MIL-125 further drove the accumulation of photogenerated electrons at Ti sites. This tandem electric field effect, in conjunction with the CO 2 adsorption and activation at Ti sites, significantly enhanced the efficiency of CO 2 reduction within the heterojunction system. The optimized photocatalyst achieving CO production at a rate of 65.6 μmol g −1 h −1 with nearly 90 % selectivity without the use of sacrificial agents, exhibiting a remarkable 43-fold and 8-fold enhancement in activity compared to pristine MIL-125 and BiOBr, respectively. In-situ infrared spectroscopy and theoretical calculations confirmed the energy optimization effect of the heterostructure on CO 2 activation and the hydrogenation reaction, facilitating the formation of the key intermediate *COOH. This work elucidates the mechanism by which tandem built-in electric fields facilitate charge separation.
研究领域:
材料科学
·
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
POLYHEDRON
·
2023
·
IF 2.6
Yadan Ma,Xuefen Jiang,Zhongmin Liu,Longlong Geng,Xiao lei Zhang,Ping Niu,Xiuling Zhang,Yongzheng Zhang,Dashuai Zhang,Hui Hu,Xin Li,Xiaoli Wang
Developing new adsorbents with hierarchical pore and unsaturated adsorption sites are highly demanded to achieve rapid adsorption rate and good adsorption selectivity in purifying organic wastewater. We here reported a new Quasi-MIL-125(Ti) synthesized at 340 °C under air atmosphere and considered as a high-efficiency adsorbent for capturing cationic dyes. The morphology of the material is characterized by XRD, SEM, TEM, etc. and the adsorption performance of Quasi-MIL-125(Ti) was systematically studied. Remarkably, it takes only 1 min to rapidly remove 20 mg L -1 MB or NR with 1 g L -1 Quasi-MIL-125(Ti), which is far superior to the previously reported materials. Adsorption isotherm shows that dyes adsorption on Quasi-MIL-125(Ti) follow a Langmuir adsorption isotherm model. The experimental maximum adsorption capacities were 109.3 mg g -1 for MB and 151.1 mg g -1 for NR, respectively. The hierarchical pores facilitate the diffusion and co-adsorption of different dye molecules. Adsorption mechanism reveals that the strong electrostatic attraction originated from the unsaturated Ti sites in Quasi-MIL-125(Ti) contributes to the ultra-fast adsorption behavior during cationic dyes chemisorption process. This study not only provides a promising prospect for the synthetic strategy of super-adsorbents, but also provides reference and theoretical guidance for practical dye wastewater treatment.
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Xuliang Deng,Yang Xu,Jincheng Liu,Dong Lin,Ze Zong,Juncong Yuan,Zhiyang Li,Guanghui Zhao,Yongjun Zhang,Yibin Liu,Xiaobo Chen,Xiang Feng,De Chen,Chaohe Yang,Honghong Shan
Regulating the Ti active sites in titanosilicates with different coordination modes is of prime scientific and industrial significance to the rational design of efficient catalysts for olefin epoxidation. In this study, the Ti species in Ti-beta zeolite catalysts (open/closed tetra-coordinated Ti sites, hexa-coordinated Ti species, and TiO2) were keenly controlled via the dealumination-metallization approach. By multiple characterizations, kinetics study, and multivariate model analysis, it is found that the open tetra-coordinated framework Ti(OH)(OSi)3 species contribute more to the catalytic performance for 1-hexene epoxidation with H2O2. Moreover, the Ti-beta with rich open tetra-coordinated Ti(OH)(OSi)3 species showed significantly improved reaction performance (TON: 401, conversion: 64%, selectivity: 98%, H2O2 efficiency: 97%) with lower apparent activation energy. This study not only opens up new prospects for the design of efficient titanosilicates by modifying Ti microenvironments but also proposes the strategy to improve the content of open tetra-coordinated Ti sites.
研究领域:
催化
·
材料科学
·
化学工程
·
无机化学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2024
·
IF 5.6
Zheng Bo,Mengyu Cao,Yaolin Wang,Jianhua Yan,Kefa Cen,Xin Tu
Plasma catalytic CO 2 hydrogenation has emerged as a promising approach for converting CO 2 into valuable chemicals such as CO, offering a potential solution to mitigate greenhouse gas emissions. In this study, we investigate the synergistic effect between plasma and a Cu/Ti 3 C 2 T x MXene catalyst for CO 2 hydrogenation via the reverse water gas shift (RWGS) reaction in a dielectric barrier discharge (DBD) reactor. Our findings reveal a significant enhancement in CO 2 conversion (33.1%) and CO yield (31.9%) when using the Cu/Ti 3 C 2 T x catalyst compared to plasma alone or with a Ti 3 C 2 T x foam. Plasma treatment creates unsaturated Ti sites on the Ti 3 C 2 T x surface, dramatically improving CO 2 adsorption and activation, while Cu nanoparticles significantly enhances the activation and dissociation of H 2 molecules on the catalyst surface. These surface adsorbed hydrogen species readily hydrogenate adsorbed CO 2 molecules through the Langmuir-Hinshelwood mechanism. Furthermore, these surface hydrogen species can also participate in the conversion of gas-phase CO 2 molecules through the Eley-Rideal pathway. This work sheds light on the synergistic plasma catalytic mechanism and provide insights for optimizing CO 2 hydrogenation processes using MXene catalysts.
研究领域:
化学工程
·
催化
·
环境科学
·
等离子体化学
✓ 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）