ACS Sustainable Chemistry & Engineering
·
2025
·
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
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2024
·
IF 5.8
Chaorong Chen,Haiyang Xian,Jing Liu,Qingze Chen,Xiaoliang Liang,Runliang Zhu,Michael F. Hochella
Photochemical and adsorptive reactions occurring at the mineral–water interface are of great importance in controlling the fate and transport of contaminants in nature, but the effects of the mineral surface structure on the interplay of these two processes and the underlying mechanisms remain largely unknown. In this work, two different structurally well-defined hematite nanocrystals were employed to explore the coupled photoreduction and immobilization of Cr(VI) on various facets of hematite under light irradiation. Compared with hematite quasi-nanocubes (HNCs) exposing only {012} facets, hematite nanoplates (HNPs) with exposed {001} and {113} facets exhibited higher immobilization ability for Cr(VI) under light irradiation, indicating that the coupled process of photoreduction and adsorption of Cr(VI) strongly relied on the particularly exposed facets of hematite. X-ray photoelectron spectroscopy measurements indicated that the removed Cr(VI) from solution was mainly immobilized on hematite surfaces in the form of Cr(III) (the reduced products of Cr(VI)). Transmission electron microscopy and electron energy-loss spectroscopy results revealed that the accumulation of Cr species was predominantly on the {113} facets of HNPs and the {012} facets of HNCs. Theoretical calculations show that the work function difference between the {113} and {001} facets was directly linked with the effective separation of photogenerated electron–hole pairs in HNPs, which is beneficial for the reduction of Cr(VI). The results of desorption experiments indicate that the coupling of photoreduction and adsorption processes significantly promotes the long-term immobilization of Cr species and effectively reduces their environmental risks (the desorption of Cr(VI) from the HNP and HNC samples decreased from 35.9% and 33.5% to 0.3% and 1.7%, respectively). Overall, the exposed facets can significantly affect the electron transfer properties of hematite as well as the binding affinity for Cr species, thereby governing the reduction and immobilization behavior of Cr(VI) on various facets of hematite. These results advance our understanding of the speciation and immobilization of redox-sensitive contaminants at the surfaces of semiconducting minerals in nature.
研究领域:
环境科学
·
表面化学
✓ 已验证
产品关联
DOI
高影响因子
PNAS Nexus
·
2023
·Vol. 2
·期 11
·
IF 0
Ge Qiuyue,Liu Yangyang,You Wenbo,Wang Wei,Li Kejian,Ruan Xuejun,Xie Lifang,Wang Tao,Zhang Liwu
The origin of life on Earth is an enigmatic and intricate conundrum that has yet to be comprehensively resolved despite recent significant developments within the discipline of archaeology and geology. Chemically, metal-sulfide minerals are speculated to serve as an important medium for giving birth in early life, while yet so far direct evidence to support the hypothesis for the highly efficient conversion of inorganic carbon into praxiological biomolecules remains scarce. In this work, we provide an initial indication that sphalerite, employed as a typical mineral, shows its enormous capability for promoting the conversion of inorganic carbon into elementary biomolecule formic acid (HCOOH) in airborne mineral-bearing aerosol microdroplet, which is over two orders of magnitude higher than that of the corresponding conventional bulk-like aqueous phase medium in the environment (e.g. river, lake, sea, etc.). This significant enhancement was further validated by a wide range of minerals and clays, including CuS, NiS, CoS, CdS, MnS, elemental sulfur, Arizona Test Dust, loess, nontronite, and montmorillonite. We reveal that the abundant interface of unique physical–chemical features instinct for aerosol or cloud microdroplets reduces the reaction energy barrier for the reaction, thus leading to extremely high HCOOH production (2.52 × 1014 kg year−1). This study unfolds unrecognized remarkable contributions of the considered scheme in the accumulation of prebiotic biomolecules in the ancient period of the Earth.
研究领域:
化学
·
生物学
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地球科学
✓ 已验证
DOI
PubMed
SEPARATION AND PURIFICATION TECHNOLOGY
·
2017
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IF 3.359
Fuhai Li,Yun Shang,Zuoming Ding,Hanqin Weng,Jiaxin Xiao,Mingzhang Lin
The extraction and separation of platinum group metals (PGMs) from HLLW is of great value for resource recycling and the running of reprocessing plants. In this paper, the photochemical method was proposed to extract and separate PGMs (Pd, Ru) from simulated high level liquid wastes (HLLW). Pd and Ru metal were extracted from aqueous solution by photoreduction with high efficiency (reduction ratio >90%) in the presence of alcohols, which was confirmed by UV–vis spectroscopy, XRD, XPS and TEM analysis. The effects of various parameters such as exposure wavelength, reducing agents, Cl − and pH value were investigated to optimize the photoreaction. The highly efficient extraction and separation of Pd or/and Ru metal from their mixture with lanthanide (Nd) by selective photoreduction was realized. The results suggest that the photochemical method is a promising method for the efficient extraction and separation of PGMs from HLLW.
研究领域:
化学
·
核能工程
·
环境科学
✓ 已验证
DOI
高影响因子
Carbon Letters
·
2023
·Vol. 33
·期 5
·1395-1406
·
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
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Runming Wang,Gang Cheng,Zan Dai,Jie Ding,Yunling Liu,Rong Chen
A general ionic-assisted microwave-ultrasonic combined synthetic strategy was developed to fabricate Bi 2 E 3 (E = S, Se, and Te) hierarchitectures. To understand the crystal phase transformation and morphological evolution of Bi 2 S 3 hierarchical nanostructures, the fabrication of Bi 2 S 3 hierarchitectures was investigated by varying sulfidation time and chlorination time. A topotactic transformation from BiOCl microsphere to Bi 2 S 3 hierarchitectures was proposed. It was found that the structure, size, and morphology of Bi 2 S 3 hierarchitectures could be delicately engineered by varying chlorination time, alkyl chain length, and concentration of ionic liquid. Moreover, the as-prepared Bi 2 S 3 hierarchitectures displayed superior capacity of Cr(VI) photoreduction to P25 and irregular Bi 2 S 3 nanostructures under visible light irradiation. Effects of morphology, pH value of reaction system, Cr(VI) concentration, and catalyst dosage on the Cr(VI) photoreduction capacity of Bi 2 S 3 hierarchitectures were also discussed. The enhancement of photoreduction capacity is not only attributed to the intrinsic good electron transfer ability of Bi 2 S 3 , but also to synergetic effects of special architectures, wide photoresponse range, high light photoadsorption, high BET surface area and good electron-hole separation performance. The systematic condition experiments and Cr(VI) photoreduction in electroplating and tannery wastewater experiments further demonstrated that the hierarchical Bi 2 S 3 nanospheres can be used in the actual Cr(VI)-containing wastewater treatment.
研究领域:
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
ENVIRONMENTAL POLLUTION
·
2018
·
IF 4.358
Jian Zhang,Wei Li,Ying Li,Lixiang Zhou,Yeqing Lan
Schwertmannite (SCH) has strong adsorption ability to As(III). However, there are few reports on the stability of SCH load with As(III) (SCH-As(III)). In this study, the effects of tartaric acid (TA), pH and coexisting ions including K + , Ca 2+ , Al 3+ and CO 3 2− on the photoreductive dissolution of SCH- As(III) and the release of the adsorbed As (III) were investigated. The results showed that under UV irradiation TA could greatly enhance the release of total Fe and total As from SCH-As(III). Nevertheless, the total Fe and total As in the solution decreased when TA was consumed up. Compared to SCH, the reductive dissolution of SCH-As(III) was obviously suppressed. In the dark, TA could slowly enhance the dissolution of SCH-As(III), but its effect on the release of adsorbed As(III) was weak. Low pH was conducive to the release of iron and arsenic. Ca 2+ , K + , and CO 3 2− promoted the decrease of the dissolved total Fe in the later reaction. However, Al 3+ inhibited the decrease of the dissolved total Fe and total As. The analyses of FTIR and XRD demonstrated that the mineralogical phase of SCH-As(III) after reaction changed. With light, the dissolved total Fe and total As existed mainly as Fe(II) and As(V), respectively. This is because Fe(II) was generated via ligand to metal charge transfer and As(III) was oxidized to As(V) by ·OH produced during the reaction. Thus, this study provides us with a comprehensive understanding of the stability of SCH-As(III) and the release of adsorbed As(III) in natural environments.
研究领域:
环境科学
·
矿物学
✓ 已验证
DOI
PubMed
高影响因子
Catalysts
·
2025
·Vol. 15
·期 5
·460
·
IF 4
Yameng Wang,Ao Xu,Jihui Lang,Bin Zuo,Zihan Yu,Keyu Cui,Xuefei Li,Kewei Zhang,Xin Li,Maobin Wei,Jian Cao
CO2photoreduction technology offers significant potential for addressing energy and environmental challenges, though its practical application is hindered by insufficient photo-absorption and rapid carrier recombination. Herein, we constructed the WO3/In2S3S-scheme heterojunction through hydrothermal assembly of two-dimensional WO3nanosheets and scale-like In2S3nanoflakes. Systematic characterization via XRD, XPS, SEM, and TEM verified the successful preparation of hierarchical nanostructures with optimized interfacial contact in the WO3/In2S3composites. UV-Vis DRS analysis showed that the photo-absorption range of the catalyst was significantly widened. Photoelectrochemical investigations (EIS, TPR, PL, and LSV) revealed enhanced carrier separation efficiency and reduced recombination kinetics in the heterojunction system. The optimized WO3/In2S3(WI-60) catalyst had a CO evolution efficiency of 55.14 μmol·g−1under the UV-Vis light, representing a 3.9-fold enhancement over the pure In2S3(14.08 μmol·g−1). Mechanistic studies through the XPS and band-structure analysis confirmed the establishment of an S-scheme carrier’ transfer pathway, which simultaneously preserved strong redox potentials and promoted the separation process of carriers. This research provides a validated strategy for developing efficient S-scheme photocatalytic systems for solar fuel generation.
研究领域:
材料科学
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环境科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
Nanomaterials
·
2020
·Vol. 10
·期 11
·2206
·
IF 4.324
Gaoqian Yuan,Gen Zhang,Kezhuo Li,Faliang Li,Yunbo Cao,Jiangfeng He,Zhong Huang,Quanli Jia,Shaowei Zhang,Haijun Zhang
Loading a noble metal on Bi4Ti3O12could enable the formation of the Schottky barrier at the interface between the former and the latter, which causes electrons to be trapped and inhibits the recombination of photoelectrons and photoholes. In this paper, AgPt/Bi4Ti3O12composite photocatalysts were prepared using the photoreduction method, and the effects of the type and content of noble metal on the photocatalytic performance of the catalysts were investigated. The photocatalytic degradation of rhodamine B (RhB) showed that the loading of AgPt bimetallic nanoparticles significantly improved the catalytic performance of Bi4Ti3O12. When 0.10 wt% noble metal was loaded, the degradation rate for RhB of Ag0.7Pt0.3/Bi4Ti3O12was 0.027 min−1, which was respectively about 2, 1.7 and 3.7 times as that of Ag/Bi4Ti3O12, Pt/Bi3Ti4O12and Bi4Ti3O12.The reasons may be attributed as follows: (i) the utilization of visible light was enhanced due to the surface plasmon resonance effect of Ag and Pt in the visible region; (ii) Ag nanoparticles mainly acted as electron acceptors to restrain the recombination of photogenerated electron-hole pairs under visible light irradiation; and (iii) Pt nanoparticles acted as electron cocatalysts to further suppress the recombination of photogenerated electron-hole pairs. The photocatalytic performance of Ag0.7Pt0.3/Bi4Ti3O12was superior to that of Ag/Bi4Ti3O12and Pt/Bi3Ti4O12owing to the synergistic effect between Ag and Pt nanoparticles.Keywords:photocatalytic;Rhodamine B;photoreduction;Bi4Ti3O12;AgPt/Bi4Ti3O12
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2017
·
IF 9.446
Yaru Li,Zhongmin Liu,Yongchuan Wu,Jitao Chen,Jingyu Zhao,Fengmin Jin,Ping Na
Carbon dots-TiO 2 nanosheets (CDs-TNs) composites were synthesized by hydrothermal method and applied for the first time in photoreduction of Cr(VI) under sunlight illumination. The materials were characterized by transmission electron microscope, X-ray diffraction, thermogravimetric analysis, Fourier transform infrared spectrometer, and X-ray photoelectron spectroscopy analysis. The results confirmed that CDs are successfully incorporated with TNs through Ti O C bonds. With the introduction of CDs, CDs-TNs composites exhibit excellent photoreduction performance of Cr(VI), which is higher than that of TNs, P25 and CDs-P25. The unique upconversion property and electron transfer property of CDs play essential roles on light harvesting and charge carriers transferring in the photoreduction process. Most importantly, CDs could facilitate the formation of H 2 O 2 , leading to the consumption of holes. As a result, the recombination of photoinduced electron-hole pairs is hindered and photoreduction activity of CDs-TNs is promoted.
研究领域:
材料科学
·
环境科学
·
光催化
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 11
·1429
·
IF 4.501
Yali Song,Huan Zhang,Ziyan Li,Long Huang,Junhao Xie,Long Han,Ruoying Zheng,Yuqing Zhang,Hongzhong Zhang
Previous studies have displayed various conclusions about the effect of preparation factors on the photoreduction property of ZnIn2S4. Therefore, it is not easy to figure out the optimal preparation conditions of ZnIn2S4for Cr(VI) photoreduction. To ensure Cr(VI) reduction efficiency, various ZnIn2S4photocatalysts were prepared in different solvents (i.e., water and ethylene glycol) and temperatures (i.e., 120 °C, 150 °C and 180°C). Different characterization methods were used to explain the difference in optical performance and photocatalytic property among the obtained samples. The results show that all the samples exhibit a similar band gap. The reaction solvent and temperature have a great influence on the surface morphology and optical property, leading to the different photocatalytic properties. ZnIn2S4synthesized at 120 °C in the solvothermal condition shows the optimal efficiency on Cr(VI) photoreduction due to the effective utilization of photo-induced carriers. The reasonable analysis and effective conclusion presented may provide the optimal synthesis method of ZnIn2S4to effectively remove Cr(VI) from water environment.Keywords:ZnIn2S4;Cr(VI);solvothermal;hydrothermal;photoreduction
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Hanqin Weng,Yi Wang,Fuhai Li,Yusa Muroya,Shinichi Yamashita,Sheng Cheng
Recovery of platinum group metals (PGMs) including palladium (Pd), rhodium (Rh), and ruthenium (Ru) from high-level radioactive liquid waste (HLLW) possesses enormous environmental and economic benefits. A non-contact photoreduction method was herein developed to selectively recover each PGM from HLLW. Soluble Pd(II), Rh(III), and Ru(III) ions were reduced to insoluble zero-valent metals and separated from simulated HLLW containing neodymium (Nd) as a representative for lanthanides , another main component in HLLW. Detailed investigation on the photoreduction of different PGMs revealed that Pd(II) could be reduced under 254- or 300-nm UV exposure using either ethanol or isopropanol as reductants. Only 300-nm UV light enabled the reduction of Rh(III) in the presence of ethanol or isopropanol. Ru(III) was the most difficult to reduce, which was only realized by 300-nm UV illumination in isopropanol solution. The effects of pH was also studied, suggesting that lower pH favored the separation of Rh(III) but hindered the reduction of Pd(II) and Ru(III). A delicate three-step process was accordingly designed to achieve the selective recovery of each PGM from simulated HLLW. Pd(II) was reduced by 254-nm UV light with the help of ethanol in the first step. Then Rh(III) was reduced by 300-UV light in the second step after the pH was adjusted to 0.5 to suppress the Ru(III) reduction. In the third step, Ru(III) was reduced by 300-nm UV light after isopropanol was added and the pH was adjusted to 3.2. The separation ratios of Pd, Rh, and Ru exceeded 99.8%, 99.9%, and 90.0%, respectively. Meanwhile, all Nd(III) still remained in the simulated HLLW. The separation coefficients between Pd/Rh and Rh/Ru exceeded 56,000 and 75,000, respectively. This work may provide an alternative method to recover PGMs from HLLW, which minimize the secondary radioactive wastes compared with other approaches.
研究领域:
环境科学
·
核化学与放射化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）