ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Zhixiong Yang,Bo Hu,Xiaotian Wang,Dmitry Selishchev,Gaoke Zhang
The development of high-performance photocatalysts is crucial for enabling efficient CO2 conversion in photocatalytic systems. Here, we developed a novel heterojunction (N-BON) composed of Ni-doped Bi4O5Br2 and NiCo2O4 for CO2 photoreduction with the help of simulated sunlight. The optimized 21N-BON composite exhibited the highest activity, producing 18.66 μmol·g–1·h–1 of CO with a selectivity of 95.7%, which represents a remarkable 2.15-fold and 4.75-fold increase in CO yield compared to the Bi4O5Br2/NiCo2O4 heterojunction and Ni-doped Bi4O5Br2, respectively. Photoelectrochemical testing, photoluminescence analysis, and theoretical calculations demonstrated that the enhanced performance of the 21N-BON composite is attributed to improved photogenerated carrier separation, driven by the synergistic effects of Ni-doping-induced spin polarization and the built-in electric field from heterojunction construction. Additionally, theoretical calculations and in situ DRIFTS analyses was used to clarify the CO2 reaction mechanisms on the photocatalyst surface, showing that Ni doping improved CO2 adsorption and promoted the formation of key reaction intermediates. This study offers important guidance for developing advanced photocatalysts for solar-driven CO2 reduction, contributing to sustainable energy solutions.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
Carbon Letters
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2023
·Vol. 33
·期 5
·1395-1406
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IF 4.5
Chen Zhangjing,Li Liangliang,Cheng Gang
Photocatalytic CO 2 reduction is a promising approach for reducing CO 2 emissions and achieving the goal of carbon neutrality. In this work, selectively coupling Cu(OH) 2 and CuO with amine-modified brookite TiO 2 (NH 2 –B–TiO 2 ) has been achieved by a simple precipitation method. The results show that CuO is better than Cu(OH) 2 as a co-catalyst to enhance the CO 2 photoreduction capability of NH 2 –B–TiO 2 . The highest rates of CO 2 conversion to CH 4 and CO of NH 2 –B–TiO 2 –CuO composite reach 6.05 and 3.25 μmol h −1 g −1 , respectively, which is higher than 8 times the yield of CH 4 of NH 2 –B–TiO 2 . It is proposed that the NH 2 –B–TiO 2 –CuO composite offers an effective charge transfer through the formation of a p–n junction between NH 2 –B–TiO 2 and CuO interfaces, while in the NH 2 –B–TiO 2 –Cu(OH) 2 composite, the Cu(OH) 2 dominantly serves as an electron sink to capture photo-induced electrons, promoting photo-induced carrier separation. This work provides an ingenious synthetic method for selectively anchoring Cu(OH) 2 and CuO on semiconductors with different charge transfer routes for an efficient CO 2 photoreduction. Graphical abstract
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Shujie Liang,Yan Zhang,Jingxian Cong,Jiaxin Lv,Hong Deng
Designing and fabricating nanozymes with photoactivity for CO 2 reduction poses a significant challenge. Here, a hierarchically structured ZFs-tpyNi heterojunction nanozyme, comprising a terpyridine-based Ni complex supported on ZrO 2 nanoframes, has been created through an interfacial engineering strategy for efficient CO 2 reduction under visible light. Due to its unique structural and compositional advantages, ZFs-tpyNi demonstrates superior photocatalytic CO 2 -to-CO conversion compared to its counterpart of ZFs and tpyNi, achieving a CO yield of 18.2 µmol and a selectivity of 92.4 % with a high apparent quantum efficiency of 0.96 % in 3 h. These innovative catalysts also show excellent durability for at least eight cycles without a loss in performance, maintaining a remarkable structural stability with no obvious collapse of its framework and morphology. Systematic investigations reveal that ZFs-tpyNi heterostructures exhibit a high specific surface area advantageous for the effective loading of tpyNi and exposure of active sites. The robust ZFs framework, characterized by extensive porosity, prevents nanoparticle agglomeration and accelerates mass transfer during catalysis. Additionally, the spatially heterogeneous interface enables precise modulation of band alignment and bandgap dynamics in nanozymes, enhancing light absorption and promoting the generation and separation of photogenerated charge carriers. Consequently, the nanozyme demonstrates enhanced CO 2 adsorption and activation capabilities, leading to improved selectivity of catalytic products. This work aims at highlight the role of nanozyme catalysts in sustainable energy production.
研究领域:
材料科学
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催化化学
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环境科学
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DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Wenchao Shangguan,Guoqiang Li,Shidi Gui,Xiaodong Zhang,Sugang Meng,Shifu Chen,Yingxuan Li
Separating photoexcited holes in metallic nanostructure to drive H 2 O oxidation reaction to balance the CO 2 photoreduction reaction is highly desirable, but challenging. The bottleneck lies in the sluggish kinetics of both photoexcited hole transfer and H 2 O oxidation. Herein, this work demonstrates that the in situ reconstruction of n -type wide-bandgap AlOOH-supported Au nanoparticle heterogeneous photocatalyst, triggered by thermal and photothermal cooperative effect during photocatalytic reactions, facilitates the efficient CO 2 photoreduction through optimizing the Au 5 d -band holes separation and H 2 O activation. In situ and ex situ characterizations evidence restructuring at interfaces to form an ultrathin γ-Al 2 O 3 nanolayer (≈2 nm thickness), which optimizes the energy band structure and promotes spontaneous transfer of photoexcited Au 5 d -band holes to the valence band of AlOOH, and prolongs the lifetime of electrons available for CO 2 reduction on Au. Furthermore, hydroxyl vacancies generated during restructuring process are demonstrated to promote H 2 O adsorption and lower the energy barrier for O 2 formation, supplying adequate protons for CO 2 protonation reduction and thereby boosting CO 2 photoreduction efficiency. This study offers valuable insights into the underlying mechanisms of utilizing n -type semiconductors to separate photoexcited d -band holes in metal nanoparticles.
研究领域:
材料科学
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催化化学
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环境科学
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DOI
高影响因子
Jove-Journal of Visualized Experiments
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2019
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IF 1.108
XiaoXiang Fang,Zhihong Gao,Hanfeng Lu,Qiulian Zhu,Zekai Zhang
We demonstrate a method for the enhancement of CO2 photoreduction. As the driving force of a photocatalytic reaction is from solar light, the basic idea is to use concentration technology to raise the incident solar light intensity. Concentrating a large-area light onto a small area cannot only increase light intensity, but also reduce the catalyst amount, as well as the reactor volume, and increase the surface temperature. The concentration of light can be realized by different devices. In this manuscript, it is realized by a Fresnel lens. The light penetrates the lens and is concentrated on a disc-shaped catalyst. The results show that both the reaction rate and the total yield are efficiently increased. The method can be applied to most CO2 photoreduction catalysts, as well as to similar reactions with a low reaction rate at natural light.
研究领域:
环境科学
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能源化学
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DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
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IF 6.7
Junyi Qian,Hao Hu,Ying Liang,Zhijie Zhang
Halide perovskite quantum dots (PQDs) have shown great promise for the photochemical conversion of CO 2 . However, the fast carrier recombination rates and inadequate adsorption/activation for CO 2 molecules have seriously restricted their practical application. Herein, an innovative step-scheme-based Cs 2 CuBr 4 /TiO 2 (CCB/TiO 2 ) photocatalyst was prepared by embedding Cs 2 CuBr 4 PQDs in a mesoporous TiO 2 matrix, which exhibits considerable potential as candidates for CO 2 photoreduction under simulated sunlight. Remarkably, the optimised CCB/TiO 2 photocatalyst delivered an impressive CO 2 reduction activity, which was 3.1 and 16.0 times higher than those achieved by pure Cs 2 CuBr 4 and TiO 2 , respectively. Furthermore, the S-scheme charge transfer mode was comprehensively corroborated by density functional theory (DFT) calculations, photo-assisted Kelvin probe force microscopy (KPFM), in situ irradiated X-ray photoelectron spectra (XPS), and electron spin resonance spectroscopy (ESR). On basis of theoretical calculations and in situ diffuse reflectance spectra (DRIFTS), the CCB/TiO 2 exhibited a reduced energy barrier of the rate-determining step, which facilitated the CO 2 photoreduction reaction.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
Advanced Science
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2025
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IF 14.1
Fengyi Zhong,Jianping Sheng,Chenyu Du,Ye He,Fengying Zhang,Yanjuan Sun,Ying Zhou,Fan Dong
Heterojunctions, known for their decent separation of photo-generated electrons and holes, are promising for photocatalytic CO 2 reduction. However, a significant obstacle in traditional post-assembled heterojunctions is the high interfacial barrier for charge transfer caused by atomic lattice mismatch at multiphase interfaces. Here, as research prototypes, the study creates a lattice-matched co-atomic interface within CsPbBr 3 -CsPb 2 Br 5 polytypic nanocrystals (113-125 PNs) through the proposed in situ hybrid strategy to elucidate the underlying charge transfer mechanism within this unique interface. Compared to CsPbBr 3 nanocrystals, the 113–125 PNs exhibit a remarkable 3.6-fold increase in photocatalytic CO 2 reduction activity (173.3 µmol −1 g −1 within 5 h). Furthermore, Kelvin probe force microscopy results reveal an increase in the built-in electric field within this lattice-matched co-atomic interface from 43.5 to 68.7 mV, providing a stronger driving force for charge separation and directional migration. Additionally, ultrafast transient absorption spectroscopy uncovers the additional charge carrier transfer pathways across this lattice-matched co-atomic interface. Thus, this unique co-atomic interface significantly promotes the interfacial electronic coupling and mitigates the charge transfer barrier, thus facilitating efficient charge separation and transfer. These insights underscore the importance of interfacial structure in heterojunction design and comprehending the intricate interplay between interface and carrier dynamics.
研究领域:
材料科学
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化学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Xinran Li,Shuohan Li,Jian Xu,Lanxin Wang,Kaiwei Liang,Huihui Zhang,Xuelian Yu,Zhongwei Liu
Photoconversion of CO 2 into fuel is critical for realizing a net-zero emission future, but it remains an open challenge due to the unsatisfactory light absorption and photogenerated carriers’ separation efficiency of catalysts. In this work, upon in situ thermal polymerization method, the nanodiamond (ND) are homogeneously and solidly modified on the defective graphitic carbon nitride (g-C 3 N 4 ) surface. Under visible light irradiation, the ND/g-C 3 N 4 (NH) exhibits excellent CO 2 photocatalytic performance with a CO yield of 10.98 μmol/h (18.6 times higher than bulk g-C 3 N 4 ), predominant performance in the selectivity of CO and cyclic stability. The improved CO 2 photoreduction ability was sourced from the synergetic effect of nitrogen vacancies engineering and ND decoration, which also significantly improved visible light absorption capacity and facilitated electron transport pathways, and promoted the separation and transfer of charge carriers efficiently.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Bing He,Ying-Jie Wang,Xuefeng Bai,He Bian,Yabo Xie,Rui Li,Jian-Rong Li
MOF-on-MOF composites are deemed promising candidates to accomplish synergistic CO 2 capture and photoreduction thanks to their plentiful active sites, extended light response range, timely separation of photoexcited electron-hole pairs, and large CO 2 adsorption capacities. Unfortunately, the controllable growth of the designed MOF-on-MOF heterostructure is challenging. Deficient interphase contact and the consequent mass transfer deprivation is one of the primary obstacles severely impairing the catalytic efficiency. Herein, the contact between two widely-employed MOFs of Ni-BDC and NH 2 -MIL-125 was significantly strengthened by exploiting a self-assembled array of Ni-BDC microsheets. In contrast to the spontaneously formed spheroidal aggregate, the loosely-packed array exhibits amplified accessible surfaces to interact with NH 2 -MIL-125, contributing to a radically improved interfacial built-in electric field and 7∼9 times rises in the product yields. Moreover, the preferably thin thickness of Ni-BDC microsheets prompts its macroscopic flexibility, permitting intensified deformation for enhanced interphase contact. Coupled with the additional contribution from its copious Lewis acid sites, the developed NH 2 -MIL-125@Ni-BDC array simultaneously converted CO 2 into CO and CH 4 at rates that cannot be matched by its isostructural Co counterpart with declined acidity and flexibility. This work innovatively reveals the immense importance of morphology tailoring and assembly tactic to interphase contact modulation and the upgrade of catalyst performances.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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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
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环境科学
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催化化学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Shujie Liang,Jiaxin Lv,Yishun Wang,Hong Deng
The development of efficient and stable single-atom catalysts (SACs) for CO 2 photoreduction is a persistent challenge. This study reports the successful preparation of SACs by incorporating isolated Ni atoms into carbon nanorods through a low-temperature calcination process using nickel bis(dimethylglyoximate) complexes. These Ni atoms, maintaining their original coordination environments, can facilitate charge separation, and enhance CO 2 adsorption and activation. The optimized catalyst exhibits a CO formation yield of 24.4 µmol with ∼96 % selectivity in high-purity CO 2 , outperforming both the precursor and pure carbon. Additionally, the Ni SACs showed strong catalytic selectivity in diluted CO 2 conditions, with selectivity rates of 82.57 %, 80.35 %, and 61 % at 0.1, 0.05, and 0.01 atm, respectively. This work provides critical insights for designing efficient visible light-responsive CO 2 photoreduction catalysts at the atomic level.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Bo Liu,Miao Cheng,Chunyang Zhang,Yitao Si,Jiancheng Zhou,Yuqi Ren,Jie Guan,Lunbo Duan,Maochang Liu,Dengwei Jing,Naixu Li
CO 2 photoreduction into high-value-added C 2+ products struggles with energetic challenges in forming critical intermediates and multiple C−C bonds. Herein, an effectively synthesized photocatalyst , Bi 2 WO 6 nanosheets with oxygen vacancies anchoring Au and Cu dual single atoms on the surface, can convert CO 2 and H 2 O vapour into C 3 H 6 and C 2 H 4 . The high product selectivity of 18.2 % for C 3 H 6 and 65.4 % for total C 2+ hydrocarbons are achieved under concentrated light irradiation (2.4 W·cm −2 ). Au-Cu dual-single-atom sites and defect engineering strategies exhibit synergistic effects on optimizing the reaction thermodynamics and charge kinetics for CO 2 conversion. Theoretical calculations provide reference values for reaction pathways of C 3 H 6 and C 2 H 4 formation, with the C−C couplings being potential determining steps of multicarbon product formation. Our work offers a promising strategy with a combination of concentrated light irradiation technology and catalyst modification to achieve high selectivity of C 2+ products.
研究领域:
材料科学
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催化化学
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环境科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）