Catalysts
·
2025
·Vol. 15
·期 9
·892
·
IF 4
Zhen Li,Kwang Leong Choy
Electrocatalytic CO2reduction driven by renewable electricity offers a sustainable approach to producing valuable chemicals, though it is often hindered by low activity and selectivity. CuO, an important transition metal oxide, exhibits unique advantages in photoelectrocatalysis due to its high intrinsic catalytic activity and ability to serve as an active site for CO2reduction. SiO2, a widely used substrate, facilitates Cu loading and increases the specific surface area of the catalyst. Meanwhile, g-C3N4provides excellent visible-light responsiveness and efficient charge carrier mobility. Together, CuO, SiO2, and g-C3N4are earth-abundant, low-cost, and chemically stable, making them ideal for solar-to-fuel applications. Here, a novel ternary heterojunction photocatalyst was constructed using SiO2, CuO, and g-C3N4. The heterostructure significantly improves light-harvesting efficiency, promotes efficient charge separation and transport, and simultaneously mitigates photogenerated carrier recombination and catalyst corrosion. The resulting SiO2@CuO/g-C3N4catalyst demonstrates outstanding CO2conversion performance, achieving a CO yield of 17 mmolg−1h−1at 1.2 VRHEwith nearly 100% selectivity. Moreover, this work systematically investigates the electrocatalytic CO2reduction reaction (CO2RR) mechanism on Cu-based catalysts, offering insights into the formation of high-value multicarbon products and highlighting the potential of rational heterojunction design in enhancing solar-driven fuel production efficiency.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Xia Bai,Jingmin Ge,Huanhuan Yang,Huiwen Tian,Xueqi Liu,Shiying Li,Zhikun Peng,Yaxi Li,Jiahao Wang,Hongpo Liu,Qun Xu
Building of grain boundary (GB) in Cu-based catalysts has been demonstrated to be an efficient strategy to control the product selectivity of electrochemical CO 2 reduction reaction (eCO 2 RR). However, the fabrication and modulation of GBs in Cu are still challenging. In this study, a series of bare Cu catalysts with controllable density of Cu(111) GBs were investigated systematically for eCO 2 RR. These catalysts exhibit superior eCO 2 RR performance for syngas production with a high FE of ∼80 % and tunable H 2 /CO ratio of 0.46–2.78. Three-dimensional wormlike Cu with abundant (111) GBs displays a stable H 2 /CO ratio of ∼0.5 over a wide potential range from −0.9 to −1.2 V ( vs. RHE). In situ Raman and ATR-SEIRAS spectroscopy combined with DFT calculations reveal that Cu(111) GBs enhance the adsorption of CO 2 , lower the energy barriers of CO 2 to *COOH and *CO, further highlighting the potential to control syngas production with desirable proportion over Cu-based catalysts.
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 40
·2405492
·
IF 27.4
Long Jiang,Zihan Ma,Zhenjiang Gu,Peiliang Shen,Yong Tao,Weihua Li,Chi-Sun Poon
Superhydrophobic surfaces applying on concrete can greatly improve the durability of concrete by preventing the damage from water. However, traditional design of superhydrophobic concrete surfaces by external coating encounters to problems of flaking and poor surface robustness, while that by adding hydrophobic agents or particles faces the challenges of strength damage of concrete. Drawing inspiration from the carbonation phenomenon of concrete, here a new design of in situ growing superhydrophobic structures on concrete is proposed: The concrete sample is impregnated into Mg 2+ -containing silane–water system with continuous CO 2 injection. The contact angle of the concrete surface achieves 171.9° without obvious strength decrease after 120 min, which are mainly attributed to the formation of Ca x Mg 1−x CO 3 crystals with micro-nano-structures and the reduction of carbonates surface energy by silane. This superhydrophobic concrete structure can be divided into a superhydrophobic–hydrophobic–hydrophilic three layers structure, providing the stable water-proof protection under mechanical fatigue, capillary water absorption, UV aging, sulfate attack, and impurity water impact tests due to the in situ growing robust superhydrophobic structures. Furthermore, it captures 29.80 g m −2 CO 2 during the reaction process, providing new insights for the design and preparation of eco-friendly superhydrophobic concrete.
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Wanfeng Xiong,Duanhui Si,Jundong Yi,Yuanbiao Huang,Hongfang Li,Rong Cao
Multicomponent heterogeneous catalysts present excellent catalytic performance attributed to the synergistic effect of multi-sites. Nevertheless, identifying the composition of the multi-sites and exploring the synergistic catalytic mechanisms for the multiple active sites in electrocatalytic CO 2 reduction reaction (CO 2 RR) still lack intensive study. This work regulates the chemical composition of Cu-based nanoreactors readily by adjusting the geometrical morphology of metal-organic frameworks precursor. The obtained cuboctahedron nanoreactor containing Cu-N 4 /Cu 2 O/Cu multiple active sites exhibits excellent CO 2 RR selectivity towards deep reduction product (80%) with high current density. Moreover, the tandem catalytic mechanism of multicomponent active sites has been studied intensively. The CO 2 molecule is firstly reduced in Cu-N 4 sites to form CO and then the CO is transfered to Cu 2 O/Cu sites for further deep reduction. The high concentration of CO provided by Cu-N 4 sites decreases the free energy of rate-determining step for CH 4 products in Cu 2 O sites. This work provides a promising direction for designing and synthesizing multicomponent Cu-based tandem catalysts to access high efficiency and selectivity in the electrocatalytic CO 2 reduction reaction.
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Huiyan Ren,Liuliu Zhu,Hongbo Gu
Converting CO 2 into high-value C 2+ products under neutral conditions holds significant importance for both energy development and environmental sustainability, yet it remains a formidable challenge. In this work, we synthesize sea urchin-shaped Cu x O nanoparticles coated with polydopamine (Cu x O@PDA), in which the PDA creates a favorable local microenvironment for electrocatalytic CO 2 reduction reaction (ECO 2 RR). Specifically, PDA promotes the hydrogenation reduction of *CO, stabilizes the pivotal *CHO and *OCCHO intermediates, and reduces the energy barrier for the coupling of *CO and *CHO. Leveraging these advantages, Cu x O@PDA achieves a maximum Faraday efficiency for C 2 H 4 up to 53.4% in the neutral electrolyte at potential of -1.4 V vs . RHE, which is 22.3% higher than that of Cu x O at the same potential. This study offers new insights into enhancing the electrocatalytic CO 2 reduction performance of copper oxides through polymer modification, providing a promising strategy for improving the selectivity and efficiency of C 2 H 4 product under neutral conditions.
✓ 已验证
产品关联
DOI
高影响因子
Science Bulletin
·
2025
·
IF 21.1
Yiding Wang,Runyao Zhao,Jiaju Fu,Fengtao Zhang,Tianyu Yu,Linzi Wen,Yanfei Zhao,Jin-Song Hu,Buxing Han,Zhimin Liu
Cu-based catalysts have been considered promising electrocatalysts for converting CO 2 into multi-carbon products (C 2+ products). However, achieving selectivity toward a specific C 2+ product remains challenging, necessitating the delicate design of catalytic sites to regulate the energy preference of reaction pathways. Herein, we introduced catalytic sites that evolve active hydrogen atoms (*H) on Cu surfaces to regulate electrocatalytic CO 2 hydrogenation pathways to achieve the selective production of ethylene. Ru single-atom site (Ru 1 ) was theoretically screened from 17 elements with 51 structures, exhibiting optimal activity in promoting hydrogenation of CO 2 reduction intermediates. The accordingly synthesized Ru 1 -doped oxide-derived Cu (Ru 1 -ODCu) catalyst delivered an ethylene selectivity of 82% in C 2+ products with a Faradaic efficiency of 58.9% and a partial current density of 353.4 mA cm –2 in KHCO 3 electrolyte. Kinetic isotope and in situ spectroscopic analyses evidenced that the Ru 1 sites effectively promote intermediate hydrogenation by regulating *H transfer to intermediates, facilitating the energy-preferred pathway to ethylene production. These results provide insights into the design of Cu catalysts with intermediate hydrogenation sites for converting CO 2 into specific products.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yujie Tan,Ran Sun,Hui Xu,Yuan Yuan,Xingang Liu,Andrew E.H. Wheatley,Renxi Zhang
By employing a non-metal doping strategy, we systematically achieved the stabilization and synergistic modulation of both surface defects and spin polarization within the wide-bandgap semiconductor. This platform is crucial for advancing key applications in both environmental remediation and energy conversion. Optimized photocatalytic activity in TiO 2 is achieved by tailoring its electronic structure through a template-assisted route, where boron acids act simultaneously as dopants and mesopore-directing agents. Mechanistically, advanced techniques including PAS, EXAFS, OCPD and DFT calculations reveal spin polarization in TiO 2 arises when interstitial boron pairs with nearby oxygen vacancies to form B–Ov complexes that stabilize vacancy-derived defect states and, via local dipoles and distortion of TiO 6 octahedron, break spin degeneracy near Fermi level (E f ), thereby suppressing spin-allowed recombination and enhancing photocatalytic charge utilization. Notably, employing boron also enables precise control of hierarchical porosity and surface area in metal oxides. The resulting TiO 2-x bearing spin-polarized B–Ov complexes delivers CO from CO 2 at 24 µmol h⁻¹ g⁻¹ with high selectivity and degrades tetracycline under visible light within 2 h (k = 0.016 min⁻¹), which are 6- and 16-fold faster than pristine TiO 2 and TiO 2 -based photocatalysts reported under similar TC degradation conditions. This work presents a significant advance in the methodology for constructing next-generation free-standing photocatalysts.
✓ 已验证
产品关联
DOI
高影响因子
MACROMOLECULES
·
2025
·
IF 5.2
Fan Hu,Jinpeng Luo,Shichao Feng,Liangqiang Wei,Shinji Ando,Yinhua Wan,Yongbing Zhuang
Conventional polyimide (PI) membranes exhibit low H2/CO2 selectivity (≤3.1). To address this limitation, this study synthesized a novel diamine monomer, 5-amino-2-(4-hydroxy-3-aminobenzene)-benzoxazole (OH-BOA), specifically designed with benzoxazole and hydroxyl functionalities. Subsequently, OH-BOA and its structural counterpart 5-amino-2-(4-hydroxy-3-aminobenzene)-benzimidazole (OH-BIA) were copolymerized with pyromellitic dianhydride (PMDA) to yield four hydroxy-functionalized poly(benzoxazole-benzimidazole-imide)s (OH-CoPIs). These OH-CoPIs exhibited good solubility, robust mechanical properties (tensile strength ≥ 114.9 MPa), high glass transition temperatures (Tg > 400 °C), and low coefficients of thermal expansion (CTE ≤ 28.3 ppm/K). Notably, they achieved a significantly enhanced H2/CO2 selectivity of up to 12.2, surpassing the commercial Matrimid 5218 (3.1) by 4-fold. Systematic evaluation revealed that increasing benzoxazole content reduced the CTE while enhancing tensile strength, Young’s modulus, and H2/CO2 selectivity. The thermally rearranged membrane (TR-40CoPI-400, 400 °C) achieved high H2 permeability (26.00 Barrer) with optimal selectivity (7.6) and exceptional CO2 plasticization resistance. The synergistic integration of benzimidazole, benzoxazole, and hydroxyl groups enables high-performance PI membranes for H2/CO2 separation.
✓ 已验证
产品关联
DOI
高影响因子
Materials
·
2025
·Vol. 18
·期 17
·4148
·
IF 3.2
Xiang Liu,Fujiang Huang,Xiang Shi,Hangmin Xu,Jian Xu,Xingwang Zhu
Alongside the gradual progress of industrialization and the continuous development of human society, the problems of environmental pollution and energy crisis have become increasingly prominent. Semiconductor photocatalysis is a promising solution to these challenges. The photocatalytic reduction of CO2by TiO2to produce carbon monoxide and methane is a process which has been identified as a means of developing clean energy. In this paper, two-dimensional TiO2(2D-TiO2) was synthesized via a one-step solvothermal method, and one-dimensional TiO2(1D-TiO2) was obtained through a hydrothermal process. Their photocatalytic CO2reduction performances were systematically investigated. The results show that 2D-TiO2exhibits superior catalytic activity compared to 1D-TiO2, which can be attributed to its lamellar structure, larger specific surface area, and improved hydrophilicity, providing more active sites and faster reaction kinetics. To further reveal the reaction mechanism, density functional theory (DFT) calculations were carried out using VASP with the GGA–PBE functional, PAW potentials, and a plane-wave cutoff energy of 520 eV. A 3 × 3 × 1 Monkhorst–Pack grid was used for Brillouin zone integration, and all possible adsorption configurations of CO2*, COOH*, and CO* intermediates on the 2D-TiO2surface were evaluated. The results confirm that 2D-TiO2stabilizes key intermediates more effectively, thereby lowering the energy barrier and facilitating CO2reduction. These findings demonstrate that structural modulation of TiO2significantly influences its photocatalytic performance and highlight the great potential of 2D-TiO2for efficient CO2conversion and clean energy applications.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
The Innovation
·
2025
·
IF 25.7
Yaoyu Yin,Zhongnan Ling,Shiqiang Liu,Jiapeng Jiao,Meng Zhou,Pei Zhang,Xing Tong,Yueqian Fan,Jiahao Yang,Huanyan Liu,Xueqing Xing,Jianling Zhang,Yi Xu,Hongyan Liang,Xinchen Kang,Buxing Han
Ionomers play a vital role in the preparation of electrodes for CO 2 electroreduction, and controlling the ionomer configuration on the catalyst surface offers an effective strategy for adjusting the surface microenvironment of the electrode, thereby influencing the distribution of CO 2 electroreduction products. In this study, we demonstrate that Nafion, a commonly used ionomer, exhibits distinct aggregation behaviors in solvents with different dielectric constant (ε) values. These differences in aggregation result in varied Nafion arrangements on the catalyst surface, which in turn affect the binding of ∗CO and ∗H intermediates, enabling control over product distribution. For example, over a Cu nanosheet catalyst at 800 mA cm −2 , the Faradaic efficiency for multicarbon products increases from 67.5% to 90.5% simply by changing the dispersion solvent from low-ε dimethyl sulfoxide to moderate-ε isopropanol. This work introduces a novel approach for fine-tuning CO 2 electroreduction product distribution through manipulation of the dispersion solvent without requiring modifications to the catalyst or ionomer.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
·
IF 4.7
Fengming Mo,Tao Huang,Jinqiang Peng,Yaoyao Shen,Ting Wu,Yuqing Li,Fei Zhang,Xiangshu Chen,Hidetoshi Kita
ZSM-58 membranes were successfully prepared using nanosized ZSM-58 crystals as seeds via a secondary growth method. The effects of various synthesis conditions, including temperature and time, were systematically investigated to elucidate their influence on crystalline structure and morphology. The performance of the membranes synthesized by nano-crystal seeding is superior to that of the membranes synthesized by micro-crystal seeding. The results demonstrate that the ZSM-58 membrane exhibits high selectivity for CO 2 /CH 4 (142.40), CO 2 /N 2 (28.62) and CO 2 /CO (13.79). Additionally, the CO 2 permeance values for binary gas mixtures are 2.56×10 -7 mol·m -2 ·s -1 ·Pa -1 , 2.31×10 -7 mol·m -2 ·s -1 ·Pa -1 and 2.40×10 -7 mol·m -2 ·s -1 ·Pa -1 , respectively. Furthermore, under continuous operation for 100 hours with an equimolar gas mixture, the membrane's separation performance remains stable, with CO 2 permeability and CO 2 /CH 4 selectivity values of 2.42×10 -7 mol·m -2 ·s -1 ·Pa -1 and 141.53, respectively. These findings indicate that the ZSM-58 zeolite membrane possesses excellent long-term stability and holds significant potential for industrial CO 2 removal applications.
✓ 已验证
产品关联
DOI
高影响因子
Joule
·
2024
·
IF 38.6
Jun Wang,Jiajia Wang,Jianyong Feng,Yingfei Hu,Huiting Huang,Ningsi Zhang,Minyue Zhao,Wangxi Liu,Changhao Liu,Zhi Zhu,Shicheng Yan,Tao Yu,Ce Zhang,Wei Yao,Zhigang Zou,Zhaosheng Li
The primary source of oxygen in space exploration is derived from water electrolysis. Herein, we discovered a mild photochemical hydrogenation process that can convert CO 2 into carbon nanotubes (CNTs) and H 2 O by using a Co-based catalyst. Hence, astronauts can extract oxygen from CO 2 metabolism to close the oxygen recycling loop (overall reaction: CO 2 → C + O 2 ), allowing for ∼100% theoretical oxygen recovery. This photochemical technique has enabled a high turnover number (the molar ratio of C to Co) of 240 for CNT formation during a 100 h reaction in a flow reactor. The oxygen recovery efficiency reaches approximately 68% when using flowing CO 2 and H 2 , surpassing the theoretical maximum (50%) for the Sabatier reaction combined with water electrolysis at the International Space Station. The tip-growth mode of CNTs principally allows long-term oxygen recovery from CO 2 , in addition to space manufacturing of CNTs.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）