CHEMOSPHERE
·
2023
·
IF 8.8
Jing Zhao,Yu Zhang,Gang Chu
Persistent free radicals (PFRs) in biochar have been found to the transformation of organic contaminants in environment. However, there remains insufficient comprehension on the relationship of biochar aging with interfacial reactivity of PFRs to the degradation of phenolic compound in geochemical process. Herein, we studied both sorption and degradation of p -nitrophenol (PNP) on fresh and aged biochars via H 2 O 2 aging under anoxic condition . With increasing aging extent, the enhancive proportion of O-centered radicals was observed progressively as indicated by increased g factors. The aging of PS350 annihilated the presence of PFRs in aged biochars of low-temperature, weakening PFR intensity. But, the aging of PS650 supplied more O-centered radicals for aged biochars of high-temperature, enhancing PFR intensity. This caused the decreased degradation on 5%PS350 and 15%PS350 (37.7–79.6% decline), whereas the increased degradation on 5%PS650 and 15%PS650 (33.3–55.8% increase). At similar intensity and species of PFRs, more adsorbed amount on fresh and aged biochars produced more degradation of PNP. Nevertheless, when PFR intensity of PS650 was much lower than that of PS350, despite high sorption capacity of PS650, the degradation amount of PS350 and PS650 was comparable. The results indicated that the reactivity of C-centered radicals of PS650 was stronger than that of O-centered radicals of PS350 in anoxic system. Overall, the interfacial reactivity of biochars was simultaneously regulated by the sorption capacity of biochars and intensity and species of PFRs. This work provides a deep perspective to the impact of biochar aging on the interfacial reactivity of PRFs to phenolic compound, which will be beneficial to accurately predict the fate of organic contaminant in carbon-rich environment.
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Nanoscale
·
2023
·Vol. 15
·期 39
·16131-16143
·
IF 6.7
Jingzhi Wang,Mei Li,Zhiliang Jin
Dynamics and morphology play a crucial role in the field of photocatalytic hydrogen production. Regulating the transfer of photogenerated charges is an effective way to improve the catalytic activity. In this paper, 1T-WS2 is introduced into a p–n heterostructure, ZnCdS/NiV-LDH, as a metalloid electron pump to transfer photogenerated electrons from semiconductors with larger work functions to metalloid materials with smaller work functions, effectively to attract photogenerated electrons, and promote charge rearrangement at the p–n heterostructure interface, so as to achieve the best utilization efficiency of photogenerated charges. Second, adjusting the morphology to increase the light absorption area of the catalyst is also a way to improve the photocatalytic activity. Two different nanosheet structures dispersed heavily stacked ZnCdS, increasing the light absorption area of the system. The optimal catalyst ratio achieves a hydrogen evolution rate of 22.37 mmol g−1 h−1, achieving 7.98% AQE and 2.12% STH conversion efficiency at 450 nm. The potential mechanism was demonstrated through in situ XPS. This study provides new insights into adding “electron pumps” to heterostructures to enhance photocatalytic activity.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Zi-Chun Fan,Xiang Bai,Xian-Yong Wei,Xing Fan,Yierxiati Dilixiati,Zhuang Li,Qian-Qian Kong,Ji Zhao,Li Li,Jia-Hao Li,Zhi-Min Zong
The efficient and clean utilization of low-rank lignite conforms the strategy of carbon neutral development. Herein, a two-step strategy of hard template method and co-precipitation method was designed to prepare nickel nanoparticles supported on mesoporous carbon (Ni x /MPC) using the residue from the ethanolysis of Longquan lignite for quantitative detection of p -nitrophenol (NP). The electrochemical reduction properties of modified glassy carbon electrodes (GCEs) with different nickel loadings ( x = 10, 15, and 20 wt%) for NP were compared, in which Ni 15 /MPC/GCE stood out and presented better conductivity, larger electrochemical active surface area, and faster electron transfer rate. According to the differential pulse voltammetry detection results, Ni 15 /MPC/GCE displays satisfactory detection limit (1.8 µM) and far wider detection concentration range (170 ∼ 10000 µM) than other reported electrochemical sensors. Moreover, Ni 15 /MPC/GCE exhibits acceptable stability and reproducibility, and the relative standard deviation of NP detection current is only 0.71% under the interference of 100-fold concentration interfering substances. Hence, the constructed Ni 15 /MPC/GCE demonstrates a promising electrochemical sensor for detecting NP in environmental sewage.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Guojuan Qu,Peng Jia,Tao Zhang,Shuai Tang,Md. Nahid Pervez,Yixiong Pang,Bin Li,Chengjin Cao,Yaping Zhao
Doping nonmetallic heteroatoms into carbonaceous materials is a proven strategy for enhancing peroxymonosulfate (PMS) activation in the degradation of endocrine-disrupting compounds (EDCs). Understanding the role of heteroatom doping defects and intrinsic defects (topological, vacancies, or edge defects) on PMS activation is crucial for designing more efficient carbon catalysts. Herein, we synthesized nitrogen (N) and phosphorus (P) co-doped carbon microspheres (NPCs) through the pyrolysis of aminophosphonic acid resin (D418) precursors and utilized them to activate PMS for bisphenol A (BPA) degradation. The pyrolysis temperature was found to regulate the type and degree of defects, as well as the configuration of N and P. NPC-1000 (pyrolysis temperature at 1000 °C) exhibited the highest reaction rate constant ( k ) (1.20 × 10 −1 min −1 ) with the lowest N and P doping defects and the highest intrinsic defect intensity resulting from the removal of N and P during pyrolysis. Density functional theory (DFT) calculations and correlation analysis between defect sites and k suggest that the adsorption of PMS was facilitated by graphitic N-coordinated C and intrinsic defect sites rather than P doping defect sites, resulting in the degradation of BPA through electron transfer and radical mechanisms, specifically superoxide radicals (O•–2). Excess halide anions led a significant increase of k with only a limited formation of trichloromethane (TCM) (disinfection byproducts) in presence of 100 mM Cl − . This research offers fundamental insights into constructing intrinsic defects through regulating heteroatom configuration, intending to enhance the catalytic activity of metal-free materials.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Peng-Fang Zhang,Jia-Hui Li,Shao-Jian Zhang,Da-Cheng Li,Su-Yuan Zeng,Shu-Ling Xu,Qing-Xia Yao,Ling-Yang Liu,Lei Ding,Heng-Xiang Li,Yi-Yang Hu,Jun-Tao Li,Yao Zhou
Zn–iodine (I 2 ) battery, as a promising energy storage device, especially under high I 2 loading, is harassed by the shuttle effect of the soluble polyiodide intermediates. Herein, the bifunctional role of 2D carbon nanosponge with rich P-dopant (4.2 at%) and large specific surface area (1966 m 2 g −1 ) in anchoring I 2 /I x − ( x = 1, 3 or 5) and catalyzing their mutual conversion is reported. Both experiment and computational results reveal the transfer of electrons from the P-doped site to iodine species, showing strong interfacial interaction. When being used as a host, it possesses high specific capture capacity for I 2 (3.34 g iodine g −1 or 1.6 mg iodine m −2 ) and I x − (6.12 g triiodide g −1 or 3.1 mg triiodide m −2 ), which thus effectively suppresses the shuttle effect, supported by in situ UV–vis and Raman spectra. In addition to the strong interfacial interaction that favors iodine conversion, the P-doped sites can also catalyze the conversion of I 5 − to I 2 , which is the rate-determining step. Consequently, Zn–I 2 batteries under a high I 2 content (70 wt%) deliver high specific capacity (220.3 mAh g −1 ), superior Coulombic efficiency (>99%), and low self-discharge rate; moreover, they can also operate steadily at 2 A g −1 with ignorable capacity decay for 10 000 cycles.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 32
·15089-15098
·
IF 3.3
Qixuan Qin,Na Liu,Yan Zhang,Weiyi Bu,Zhijie Zhou,Changhua Hu,Xiaohong Chuai
The sensitivity and selectivity of semiconductor metal oxides can be effectively improved by transition metal doping and noble metal loading. In this work, Ag-loaded p-type Zn-doped Fe2O3 (Ag@Zn–Fe2O3) nanoparticles were synthesized by a combination of a one-step hydrothermal route and a co-precipitation method. The prepared Ag@Zn–Fe2O3 nanoparticles show a peanut-like structure with a size of about 50–150 nm. The Zn doping and the Ag loading can synergistically improve the response of the Fe2O3 nanoparticles to acetone. At the optimum operating temperature (150 °C), the response of the Ag@Zn–Fe2O3 sensor to 100 ppm acetone is 50.2, which is significantly higher than 8.9 and 25.8 corresponding to Fe2O3 and Zn–Fe2O3, respectively. In addition, the Ag@Zn–Fe2O3 sensor exhibits excellent selectivity, good moisture resistance, and long-term stability to acetone. Meanwhile, the possible mechanism of the improved acetone sensing properties is also discussed.
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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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Journal of Materials Chemistry C
·
2023
·Vol. 12
·期 4
·1386-1395
·
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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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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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Yu Liu,Xiumei Chen,Huachen Lin,Pengjie Zhou,Yulong Ying
It is an important method to enhance the electrochemical performance of metal oxide electrode by phosphorus doping in the research of high-performance hybrid supercapacitors . Herein, we obtain a P-doped carbon nanotubes (CNT)@MnCo 2 O 4 /Co 3 O 4 film by an in-situ synthesis and subsequent phosphating. By introducing P heteroatoms, the electronic structure of MnCo 2 O 4 /Co 3 O 4 can be effectively modulated, thereby improving the electrical conductivity and increasing Faraday reaction. The electrochemical tests show that the capacity and rate performance of CNT@MnCo 2 O 4 /Co 3 O 4 have been significantly improved after phosphorus doping. The P-CNT@MnCo 2 O 4 /Co 3 O 4 electrode displays an acceptable specific capacitance of 1064.4 F g −1 . Furthermore, a supercapacitor P-CNT@MnCo 2 O 4 /Co 3 O 4 //activated carbon possesses 46.4 W h kg −1 of energy density at 800 W kg −1 . After 10000 repeated tests, the device keeps 85.0 % of the original capacitance. The above results show that the P-doped CNT/metal oxide film we designed has some inspiration on the design of energy storage electrode materials.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Yanqing Cong,Qiuyu Zheng,Wanxing Wang,Yi Zhang,Shi-Wen Lv
Exploring highly efficient electrocatalysts (OER) is critical for oxygen evolution reaction . Herein, for the first time, P-doped NiCo 2 O 4 nanosheet arrays generated on nickel foam (namely P–NiCo 2 O 4 /NF) were constructed via a feasible protocol. Notably, the etching treatment can open the internal structure of ZIF-67 to offer more electrocatalytically active surface area, and obtained NiCo 2 O 4 showed great electrocatalytic performance in OER. The introduction of P can effectively reduce the charge transfer resistance of NiCo 2 O 4 and boost OER kinetics. More importantly, doping P not only improved the hydrophilicity of NiCo 2 O 4 , but also reduced its surface potentials, which provided convenience for the adsorption of OH − over P–NiCo 2 O 4 /NF electrode. As expected, the P–NiCo 2 O 4 /NF electrode with good long-term durability displayed excellent performance for OER in alkaline solution, and an overpotential of 121.6 mV was achieved at a current density of 10 mA/cm 2 . To sum up, current work can provide a meaningful reference to prepare electrocatalyst for efficient OER.
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