Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Xudong Yin,Xiaojie Sun,Yufeng Mao,Ruzhen Wang,Dehao Li,Wenyu Xie,Zhenghui Liu,Zhisen Liu
The elimination of tetracycline hydrochloride (TC-HCl) from water has attracted extensive research attention. This study hydrothermally synthesized composite photocatalysts composed of BiVO 4 microspheres containing coexisting phases of monoclinic scheelite (M-BiVO 4 ) and tetragonal zircon (T-BiVO 4 ), i.e., MT-BiVO 4 , loaded onto P-doped g-C 3 N 4 nanosheets (PCNS). Furthermore, their morphology, structure, and photoelectrochemical properties were comprehensively characterized, and the performance and stability of photocatalytic degradation of TC-HCl were examined. Additionally, the effects of humic acid (HA), coexisting anions/cations, and actual water samples on the degradation efficiency of TC-HCl were investigated, and the degradation mechanism and pathways were examined. The findings indicated that the percentage of M-BiVO 4 in MT-BiVO 4 considerably influences the photocatalytic activity of the composite catalyst. Furthermore, the excellent photocatalytic performance of 5% BVO/PCNS was attributed to the synergistic effects of P-doping the modified g-C 3 N 4 , MT-BiVO 4 isotype heterojunction effects, and the Z-scheme heterojunction constructed from MT-BiVO 4 and PCNS, which can enhance the absorption range of the visible light and accelerate the transfer and separation of charge carriers between catalysts. The free radical capture experiments and electron spin resonance tests indicated that holes and O 2 - were the dominant active species in the photocatalytic degradation process. With high reusability and stability, the 5% BVO/PCNS composite has great potential for practical wastewater treatment applications. This study offers a new approach for preparing photocatalysts synergized by isotype and Z-scheme heterojunctions.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Junjie Fu,Afei Zhang,Dongxing Kou,Zewen Xiao,Wenhui Zhou,Zhengji Zhou,Shengjie Yuan,Yafang Qi,Zhi Zheng,Sixin Wu
One important issue limiting the development of Cu 2 ZnSn(S,Se) 4 (CZTSSe) solar cells is the severe recombination loss at CZTSSe/Mo(S,Se) 2 /Mo back contact, primarily arising from the non-matched potential barrier and inferior electric contact between absorber and weak n -type Mo(S,Se) 2 interfacial layer. It is expected that a p-type Mo(S,Se) 2 can effectively improve the hole extraction and enhance the device performance. In this work, we propose a plausible direction to build up an electrically benign back surface field by in-situ doping Mo(S,Se) 2 with group VB elements (TM = V, Nb and Ta). It is turned out that the generated V Mo , Nb Mo , or Ta Mo shallow acceptors could convert Mo(S,Se) 2 from weak n -type to p-type conductivity and increase its work function ( W F ) and hole concentration. With the contact of p-type absorber ( W F,absorber < W F,Mo(S,Se)₂ ), a benign ohmic contact with favorable downward band bending is formed, thereby accelerating the holes extraction and minimizing interface recombination loss. With significant gains in open-circuit voltage ( V oc ) and fill factor (FF), the Mo(S,Se) 2 :Ta device finally increases the efficiency from 10.82 % to 12.72 %. This convenient in-situ Mo(S,Se) 2 doping strategy is different from previous complicated or unstable cases and should serve as a basis for high-quality back contact engineering in kesterite photovoltaics.
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FOOD CHEMISTRY
·
2022
·
IF 9.231
Ying Li,Rida Javed,Rui Li,Yuyang Zhang,Ziyue Lang,Hongbin Zhao,Xing Liu,Hongmei Cao,Daixin Ye
Ascorbic acid is one of the important vitamins to maintain human life activities and plays an irreplaceable role in regulating human redox metabolism. Fresh fruit can provide plenty of AA to maintain human metabolic balance. Thus, it is great significant to develop a rapid and convenient method for detection of AA to evaluate the freshness and nutritional quality of fruits. In this work, Fe single-atom nanoenzyme (Fe-SAN) based colorimetric sensor assisted with smartphone was designed for rapid and on-site AA detection in tropical fruits. Firstly, Fe-SAN with high oxidase-mimicking activity was synthesized by using green tea leaves as sources of carbon and nitrogen and NaH 2 PO 2 as P source to obtain Fe-P/N C SAN, in which P was used to reconstruct the distribution of electronic to enhance the oxidase-mimicking activity of Fe-SAN. Besides, the as-synthesized Fe-P/N C SAN with remarkable oxidase-like activities could oxidize 3,3́,5,5́-tetramethylbenzidine (TMB) to blue colored oxidized TMB. AA could inhibit the oxidation of TMB, leading to blue fading. Based on the above principle, colorimetric sensor integrated with smartphone RGB mode was fabricated and exhibited a good linear detection range (0.5–100 μM) and low detection limit of 0.315 μM for AA detection under optimal conditions. More importantly, the developed sensor could rapidly and accurately detect AA in real sample, such as pineapple, wax apple and mango. Therefore, this research provides a new cost-effective method for the efficient and exact detection of AA in tropical fruit, which has a broad application prospect.
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高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 23
·4123
·
IF 5.719
Li Zhang,Linhong Ge,Lamei Deng,Xinman Tu
Herein, CuS was incorporated with ZnS to form a novel nanocomposite via cation exchange, and the product was then employed for dual application of the colorimetric determination and photocatalytic degradation of tetracycline (TC) in water. The formed p–n heterojunction provided an improved gap width and electron mobility, which could rapidly catalyze H2O2to produce plenty of •OH, supporting a color conversion with TMB. Meanwhile, the addition of TC could lead to the further enhancement in colorimetric signal, and the distinction level was sensitive to the target amount. Additionally, under light conditions, the p-CuS/n-ZnS could produce •O2−, •OH, and h+through photocatalysis, and these ions could degrade the TC via oxidation. In the colorimetric determination of TC, the signal responses were obtained within 10 min, and the detection limit was 20.94 nM. The recovery rates were 99% and 106% for the water samples from Ganjiang river. In the photocatalytic degradation, the TC was degraded by 91% within 120 min, which was threefold that of ZnS. Meanwhile, the morphology feature of the p-CuS/n-ZnS remained after multiple uses, suggesting a favorable material stability. This strategy provides application prospects for the monitoring and control of antibiotics in water.Keywords:p–n heterojunction;tetracycline;colorimetric determination;photocatalysis;degradation
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Journal of Materials Chemistry C
·
2023
·Vol. 12
·期 4
·1386-1395
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IF 6.4
Wang Fu,Wuqi Liu,Yaju Wei,Dan Liu,Songyu Li,Di Zhao,Xiaoping Wu,Lingbo Xu,Ping Lin,Can Cui,Xuegong Yu,Peng Wang
In studies addressing contact recombination, carrier-selective contacts (CSCs) have played a key role in crystalline silicon (c-Si) solar cells resulting in a higher photoelectrical conversion efficiency (PCE). Recently, wide-bandgap metal compound materials with extreme work functions or suitable energy band alignment have drawn considerable interest for CSC materials. Among them, cuprous iodide (CuI) is a very promising hole-selective layer, however, very little research has been conducted for c-Si solar cells. In this work, we have demonstrated that solution-processed CuI films act as effective full-area hole-selective contact layers for p-Si solar cells. Moreover, iodine (I2) doping suppresses the generation of I− vacancies (VI), and enhances the film conductivity due to an increase in copper vacancies (VCu). Aluminum ion (Al3+) doping further promotes the generation of more VCu and increases the work function of the CuI film. The proposed I2 and Al3+ co-doping strategy for CuI films significantly improves the passivating contact performance of the Al3+–I2:CuI/p-Si heterojunction, contributing to the significantly improved PCE from 15.12% to 18.28%, which is the highest for solution-processed copper-based hole transport layers for c-Si solar cells to date. The results demonstrate the great potential of the CuI hole-selective layer applied for highly efficient c-Si solar cells.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
·
IF 6
Qingqin Sun,Xu Fu,Peiru Wang,Kunlan Li,Ligang Wei,Shangru Zhai,Qingda An
The oxidative depolymerization of alkali lignin (AL) catalyzed by copper-containing imidazolium-based ionic liquids ([C 4 C 1 im]CuCl 3 ) was investigated with CH 3 OH-H 2 O (9/1, v/v) as solvent under an initial oxygen pressure of 1.5 MPa at 150 °C for 3 h. Compared with other transition-metal chlorides and metal-containing ionic liquids (ILs), [C 4 C 1 im]CuCl 3 presented a relatively remarkable catalytic capacity for AL oxidative depolymerization due to the cooperative effects of [C 4 C 1 im] + and CuCl 3 − . [C 4 C 1 im]CuCl 3 molar concentration ( x McIL ) greatly influenced AL conversion and product selectivity. The highest AL conversion of 70.4% was achieved at x McIL = 0.18 mol.%. For the obtained small-molecule products, the highest selectivity of p -hydroxybenzaldehyde reached 51.3% at x McIL = 0.72mol.% (corresponding yield of 103.6 mg·g −1 ). The inter-unit linkages of lignin were effectively cleaved in the oxidative depolymerization catalyzed by [C 4 C 1 im]CuCl 3 , and the H unit in lignin was preferentially destroyed. The molecular interactions and microenvironment of [C 4 C 1 im]CuCl 3 –solvent (CH 3 OH-H 2 O) system were investigated with x McIL varied from 0.05 mol.% to 5.12 mol.% by using attenuated total reflectance-infrared spectroscopy and molecular-dynamics method, respectively. The catalytic properties of [C 4 C 1 im]CuCl 3 strongly depended on the interactions of [C 4 C 1 im]CuCl 3 and solvent molecules with changes in microstructure organization. The optimum catalytic capacity of [C 4 C 1 im]CuCl 3 was obtained when the ion pair formed through hydrogen bonding at x McIL = 0.18–0.36 mol.%. The solvation of solvent molecules on CuCl 3 − and the formation of ionic cluster with the hydrogen-bonding self-association of [C 4 C 1 im]CuCl 3 were unfavorable for the oxidative depolymerization of lignin.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·Vol. 29
·期 56
·e202301521
·
IF 4.3
Luoluo Qi,Zhiyang Huang,Miao Liao,Lei Wang,Lixia Wang,Mingcheng Gao,Tayirjan Taylor Isimjan,Xiulin Yang
Graphical A CoP−FeP heterostructure catalyst with abundant P vacancies (Vp−CoP−FeP/NF) on nickel foam is constructed through impregnation and phosphorization. It demonstrates excellent hydrogen evolution performance and has practical application prospects in high-current overall water splitting. The catalyst‘s unique hierarchical nanosheet structure, plentiful P vacancies and synergistic effect of CoP and FeP accelerate HER kinetics, resulting in its superior performance. The development of hydrogen evolution reaction (HER) catalysts with high performance under large current density is still a challenge. Introducing P vacancies in heterostructure is an appealing strategy to enhance HER kinetics. This study investigates a CoP−FeP heterostructure catalyst with abundant P vacancies (Vp−CoP−FeP/NF) on nickel foam (NF), which was prepared using dipping and phosphating treatment. The optimized Vp−CoP−FeP catalyst exerted prominent HER catalytic capability, requiring an ultra-low overpotential (58 mV @ 10 mA cm −2 ) and displaying robust durability (50 h @ 200 mA cm −2 ) in 1.0 M KOH solution. Furthermore, the catalyst demonstrated superior overall water splitting activity as cathode, demanding only cell voltage of 1.76 V at 200 mA cm −2 , outperforming Pt/C/NF (−) || RuO 2 /NF (+) . The catalyst‘s outstanding performance can be attributed to the hierarchical structure of porous nanosheets, abundant P vacancies, and synergistic effect between CoP and FeP components, which promote water dissociation and H* adsorption and desorption, thereby synergically accelerating HER kinetics and enhancing HER activity. This study demonstrates the potential of HER catalysts with phosphorus-rich vacancies that can work under industrial-scale current density, highlighting the importance of developing durable and efficient catalysts for hydrogen production.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Lulu Zhu,Baiyu Zhang,Qian Su,Runlu Liu,Jingyi Lin,Hua Wang,Shenmin Zhu,Yao Li
Photoinduced charge separation and surface reactions are essential for ensuring high quantum efficiency of the photochemical and photophysical processes. BiVO4-based heterojunctions are promising materials for high-performance photocatalysts; however, their photocatalytic performance is significantly lower than the theoretical limit due to the sluggish water oxidation dynamics and rapid recombination of charge carriers on the catalyst surface. To address these issues, oxygen vacancies (OVs) are introduced to a rationally designed BiVO4-based heterojunction using built-in potential and gradient OVs to promote the separation of carriers and increase the photocatalytic activity. The heterojunctions with OVs exhibit a 2-fold increase in the photocatalytic activity for phenol degradation compared with that of pristine BiVO4. Additionally, density functional theory is applied to elucidate the synergistic mechanism of light absorption and charge separation in BiOCl/BiVO4 p–n heterojunction photocatalysts containing vacancies. The obtained results demonstrate a synergistic effect of vacancies and the built-in potential, providing a pathway for defect engineering in photocatalytic processes.
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Materials Today Sustainability
·
2023
·
IF 7.8
Z. Hao,Q. Zhao,Y. Wang,H. Lu,X. Liu,Q. He,T. Wang,J. Wang,J. He,W. Wang
The complete removal of harmful phenolic contaminants from water remains huge challenge because of the lack of cost-effective and powerful adsorbents. Herein, a sustainable nitrogen self-doped biochar (named KBC750N) with large specific surface area (1398.44 m 2 /g), high adsorption capacity (606.06 mg/g) and removal ratio (99.99%) for p -nitrophenol (PNP) in real waters (Seawater, Yangtze River water , and Yellow River water) was prepared from a naturally abundant protein-rich psammophyte Caragana korshinskii (CK) by a facile one-step pyrolysis process . The in-situ nitrogen-doped biochar shows much better adsorption removal efficiency of 99.99% toward PNP than expensive commercial adsorbents (only 77.52%). The biochar still keeps high adsorption efficiency after reused more than five times. Site energy distribution analysis revealed that the biochar captures PNP mainly through n–π and π–π electron-donor–acceptor interactions among the electron-rich functional groups (N-containing moieties, –COOH, and –OH), graphite carbon, and PNP. Density functional theory (DFT) calculations confirmed that the nitrogen site in biochar helps to strengthen its adsorption capability to PNP. This work provides a sustainable platform for the development of high-performance, cost-effective materials for efficient elimination of organic pollutants from water.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 28
·9744-9756
·
IF 4
Yanxia Wang,Xiude Hu
The development of new, efficient noble-metal-free photocatalysts is of great significance for the photocatalytic hydrogen evolution reaction. Herein, Co9S8 with a hollow polyhedral structure was synthesized by in situ sulfurization of ZIF-67, and subsequently, Co9S8@Ni2P composite photocatalytic materials were prepared by loading Ni2P on the surface of Co9S8 through a solvothermal method based on a morphology regulation strategy. The design of the 3D@0D spatial structure of Co9S8@Ni2P is favorable for the formation of photocatalytic hydrogen evolution active sites. Due to the excellent metal conductivity of Ni2P, Ni2P as a cocatalyst can accelerate the separation of photogenerated electrons from holes in Co9S8, thus providing a large number of available photogenerated electrons for photocatalytic reactions. It is worth mentioning that a Co–P chemical bond is formed between Co9S8 and Ni2P, which plays an active role in the transport of photogenerated electrons. The densities of states of Co9S8 and Ni2P were determined by density functional theory (DFT) calculations. The reduction of the hydrogen evolution overpotential and the formation of efficient charge-carrier transport channels on Co9S8@Ni2P were confirmed by a series of electrochemical and fluorescence tests. This study provides a new idea for the design of highly active noble-metal-free materials for the photocatalytic hydrogen evolution reaction.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zhen Wang,Ying Fang,Ying Yang,Bo Qiu,Haipu Li
A rational design of high-performance catalysts with peroxymonosulfate (PMS) activation and arsenic adsorption capacities for the removal of p -arsanilic acid ( p -ASA) is in high demand but remains a significant challenge. Herein, vacancies-rich metal–organic frameworks (MOFs) were constructed by room-temperature co-precipitation procedure, and the magnetic CoFe encapsulated in N -doped carbon nanotubes (CoFe- N -CNTs) were prepared using MOFs template by an annealing process under a nitrogen atmosphere. The synthesis conditions of CoFe- N -CNTs were optimized by tuning Fe/Co ratio and carbonization temperature. The CoFe- N -CNTs/PMS system showed favorable removal performance, achieving complete degradation of 46 μM p -ASA within 3 min and a total arsenic removal efficiency of 98% within 30 min at 0.1 g/L catalyst and 400 μM PMS. The degradation rate ( k obs ) and total arsenic removal efficiency towards p -ASA by CoFe- N -CNTs/PMS system were 6.7 and 2.7 times of those in the MOFs without vacancies-derived catalyst/PMS system, respectively. CoFe- N -CNTs/PMS system exhibited robust and efficient performance over a broad range of pH (4.5–9.0) and in different water matrices. Scavenging experiments and electron paramagnetic resonance (EPR) results demonstrated that non-radical singlet oxygen ( 1 O 2 ), sulfate radicals (SO 4 − ), hydroxyl radicals ( OH), and superoxide (O 2 − ) were involved in p -ASA decomposition. Electron transfer and direct oxidative transfer process (DOTP) also contributed to p -ASA degradation. High-performance liquid chromatography coupled with inductively coupled plasma mass spectrometry (HPLC-ICP-MS) analysis indicated that the arsenic moiety was cleaved from p -ASA in the form of As(III) and then rapidly oxidized to As(V). X-ray photoelectron spectroscopy (XPS) analysis indicated the removal of inorganic arsenic followed the mechanism of the inner-sphere complex. This study highlights the in-situ synthesis of CoFe- N -CNTs with outstanding activities for catalytic degradation and arsenic removal of organoarsenicals.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jiahao Ren,Siqi Huo,Guobo Huang,Tianle Wang,Jiabing Feng,Wei Chen,Shenwei Xiao,Pingan Song
The ubiquitous application of highly flammable acrylonitrile–butadienestyrene (ABS) resin has brought great fire threat to human and environment. Unfortunately, current flame retardants often improve flame retardancy but reduce mechanical and thermal properties, seriously affecting their practical application. We herein reported novel multifunctional, high-efficiency, phosphorus and nickel co-doped graphitic carbon nitride (Ni-P-C 3 N 4 ) nanoflakes to address the trade-off between flame retardancy and mechanical/thermal properties. The addition of 2.0wt% of Ni-P-C 3 N 4 increased the initial degradation temperature and tensile strength of ABS composite (ABS/Ni-P-CN2) by 15 °C and 24.3% relative to virgin ABS, indicating its positive effect on thermal and mechanical properties. Compared with ABS, ABS/Ni-P-CN2 exhibited a notable increase in time to ignition, along with 32.4% and 33.8% reductions in peak heat release rate (PHRR) and peak smoke production rate (PSPR), demonstrating excellent anti-ignition, flame-retardant and smoke-suppressive performances. The increased fire safety was mainly due to the physical barrier effect of g-C 3 N 4 nanosheets and the catalytic charring effect of P and Ni. This work offers a novel design strategy to create multifunctional flame retardants for fabricating fire-safe polymer composites with superior thermal and mechanical properties, holding great potential in industries.
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危险品化学品经营许可证（带存储）