CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Shuzhen Yu,Yongchun Hou,Qijie Jin,Liangliang Zhu,Su Chen
As global warming and greenhouse gas emissions intensify, the scientific community is continuingly seeking effective solutions. One promising strategy known as artificial photosynthesis is proposed utilizing H 2 O as a reducing agent to transfer CO 2 into fuel. However, low O 2 production and conversion efficiency have hindered this approach in matching with natural photosynthesis. In this work, we propose a novel biomimetic photocatalyst design approach to improve the catalytic efficiency by slow photon mechanism. Our design is mainly inspired by two factors: 1) Chlorophyll, an abundant natural photosynthetic pigment, can efficiently and selectively reduce carbon dioxide and plays a key role in photosynthesis; 2) The iridoplast with a biological photonic crystal structure can significantly improve the efficiency of photosynthesis. Specifically, we couple photonic crystals and photocatalyst of sodium copper chlorophyllin (ChlCu), and binder of PVA through microfluidic blowing-spinning (MBS) to spray a composite photocatalytic film that can convert carbon dioxide and water into carbon monoxide and oxygen. By optimizing the content of ChlCu and the slow photon effect related to the bandgap position, the final CLPPs 300 -0.52% has two slow photon edges overlapping with the catalyst absorption spectrum, thus generating the maximum photon capture capability and achieving a high oxygen catalytic yield of up to 7.8 mmol g -1 h −1 . The spraying property of this material enable it to be coated on the external surfaces of other materials. This opens new possibilities of photocatalytic fabric preparation for CO 2 converting, providing new ideas of greenhouse gas capture and utilization to solve environmental problems.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Weijie Yang,Kailong Sun,Jun Wan,Yang-Ai Ma,Jiaqing Liu,Bicheng Zhu,Lin Liu,Feng Fu
The insufficient generation of oxidative active species severely limits the activity of photocatalytic aerobic oxidation for organic pollutants degradation in wastewater. Herein, transition metal phosphides (TMPs) cocatalysts, including Ni 2 P, Co 2 P, and NiCoP, were loaded on Bi 4 O 5 Br 2 nanosheets by a simple liquid assembly method. Among which, 15% NiCoP/Bi 4 O 5 Br 2 heterojunction exhibits the optimal photocatalytic activity for degrading phenolic pollutants owing to the high concentration of h + and •O 2 − active species, and it displays excellent tolerance for the inorganic ions, pH value, water matrix, and outdoor sunlight. The S-scheme charge transfer mechanism was revealed for NiCoP/Bi 4 O 5 Br 2 heterojunction, which significantly improves the separation efficiency of photogenerated charge carriers and facilitates the accumulation of active h + . Furthermore, NiCoP with high reduction potential and outstanding O 2 activation ability is served as the active site for producing •O 2 − . This work can inspire the further design of bifunctional photocatalysts for efficient photocatalytic aerobic oxidation applications.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 28
·期 68
·e202202004
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IF 5.02
Conghui Zhao,Liwei Sun,Yang Xu,Beibei Dong,Yuhong Luo,Jingde Li,Jianxin Chen,Zisheng Zhang
Graphical Iodine-doped Bi 2 GdO 4 Cl with a significantly promoted visible-light-responsive O 2 -evolving performance of 154.8 μmol ⋅ h −1 and an apparent quantum efficiency of ∼1.1 % at 420 nm is reported. The incorporation of I − ions causes the extended light absorption and promoted charge separation. Visible-light-responsive bismuth-based oxyhalide has recently attracted extensive attention, however, the promotion of its charge separation is still challenging. Herein, we introduce iodine into Bi 2 GdO 4 Cl to synthetize I-doped Bi 2 GdO 4 Cl (denoted as yI−Bi 2 GdO 4 Cl, 0≤y≤2). The incorporation of I − ions is found to enhance light absorption and to accelerate charge separation by combining various characterizations such as density functional theory calculation, photoelectrochemical test, electrochemical impedance spectroscopy, photoluminescence spectrum, and open-circuit voltage decay. The O 2 -evolving performances of 1I−Bi 2 GdO 4 Cl with optimized dopant concentration of I − ion and IrO 2 loaded 1I−Bi 2 GdO 4 Cl are tremendously enhanced by ca. 4 and 45 times compared to pristine Bi 2 GdO 4 Cl. Notably, The O 2 evolution rate reaches as high as 154.8 μmol ⋅ h −1 with an apparent quantum efficiency of ∼1.1 % at 420 nm. The synthetic iodine-doped photocatalyst remains stable after long-term photoreaction, demonstrating its potential in the field of photocatalysis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Zhaomin Chen,Zhenyu Wu,Jia Xu,Rui Zhao,Xiaoxia Han,Jiwei Jiang,Mingwang Shao,Bin Dong,Zhenhui Kang
Photochemical devices show great potential in applications ranging from electrical energy storage to future smart grids. Here, we report a metal-free composite film cell based on carbon dots (CDots) and polyaniline (PANI), which could achieve 24/7 discharge and photo-charging in seawater. CDots/PANI film cell has an open-circuit-voltage (OCV) of 0.95 V, a maximum power density of 380 mW m 2 , and the ability to discharge continuously for 40 h under solar irradiation of AM 1.5 G. It couples the reduction reaction of PANI, and the CDot-catalyzed oxygen reduction reactions (ORR) during discharge. While the light-induced CDot-catalyzed oxygen evolution reaction (OER) and the reduction reaction of PANI during charging. In particular, in-situ TPV tests were used to verify the effect of the light-induced OER and the kinetic properties of the catalyst on the charge transfer at the interface. We believe this research may provide new ideas for sustainable energy conversion and storage.
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Nanomaterials
·
2022
·Vol. 12
·期 11
·1931
·
IF 5.719
Shaohong Zang,Xiaorong Cai,Mengshan Chen,Dehong Teng,Fei Jing,Zhe Leng,Yingtang Zhou,Feng Lin
Photocatalytic water splitting is one of the promising approaches to solving environmental problems and energy crises. However, the sluggish 4e−transfer kinetics in water oxidation half-reaction restricts the 2e−reduction efficiency in photocatalytic water splitting. Herein, cobalt vanadate-decorated polymeric carbon nitride (named CoVO/PCN) was constructed to mediate the carrier kinetic process in a photocatalytic water oxidation reaction (WOR). The photocatalysts were well-characterized by various physicochemical techniques such as XRD, FT-IR, TEM, and XPS. Under UV and visible light irradiation, the O2evolution rate of optimized 3wt% CoVO/PCN reached 467 and 200 μmol h−1g−1, which were about 6.5 and 5.9 times higher than that of PCN, respectively. Electrochemical tests and PL results reveal that the recombination of photogenerated carriers on PCN is effectively suppressed and the kinetics of WOR is significantly enhanced after CoVO introduction. This work highlights key features of the tuning carrier kinetics of PCN using charge-conducting materials, which should be the basis for the further development of photocatalytic O2reactions.Keywords:photocatalysis;water oxidation;cobalt vanadates;polymeric carbon nitride
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ACS Applied Energy Materials
·
2022
·
IF 6.959
Sisi Wu,Jing Yang,Ning Qin,Yingzhi Li,Haiou Wang,Yong-Wei Zhang,Qing Wang,Zhouguang Lu
LiO2 is a critical intermediate of oxygen reduction reaction in nonaqueous Li–O2 batteries that largely determines the discharge capacity and cycling stability. Currently, functional redox mediators that can promote the solution reaction route by enhancing the solvation of LiO2 have attracted tremendous interest to increase the attainable capacity. Conversely, redox mediators that quench LiO2 and facilitate the surface reaction route receive little attention. Here, we provide an in-depth exploration of the catalytic pathway and effect of a superoxide quencher that modulates the surface growth of Li2O2. Surprisingly, the predomination of the surface reaction route by ethyl viologen helps deliver a capacity as much as that promoted by the solution reaction route. The findings of this work provide a new direction of screening and evaluating functioning redox mediators for Li–O2 batteries.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 30
·14510-14516
·
IF 3.925
Yunxian Zhang,Yongyu Pang,Dong Xia,Guoliang Chai
As a successful alternative to the complex and dangerous anthraquinone process, a simple and safe method for the efficient preparation of hydrogen peroxide is to use the electrochemical two-electron oxygen reduction reaction (2e− ORR) process. Herein, we report a facile approach to achieving metal-free nitrogen-doped carbon material electrocatalysts (N-CMCs) using cheap and easily available raw materials, which also have an excellent electrochemical 2e− ORR catalytic performance and selectivity for hydrogen peroxide (H2O2). The as-fabricated nitrogen-doped carbon material electrocatalysts (named as N-CMC-1 : 5) deliver the high H2O2 selectivity of over 80% in a wide potential range from 0.30 to 0.70 V vs. RHE, where the highest H2O2 selectivity can reach 81.4% at 0.42 V vs. RHE. X-ray photoelectron spectroscopy and electrochemical analyses reveal that the content of pyrrolic-N in the catalysts has a positive effect on the 2e− ORR activity. When the catalyst contains more pyrrolic-N, the catalyst demonstrates a better 2e− ORR performance and H2O2 selectivity in alkaline medium, as well as the long-term stability of the catalyst.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 6
·060507
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IF 4.386
Zining Man,Hao Tian,Xingbao Zhu,Yu Wang,Yuanguo Wu,Xiangyu Wen,Zhe Lü
The solid-state batteries have received widespread attention due to their excellent stability and safety, however, the low ionic conductivity and weak interface contact always restricted its performance. In this work, we propose an in situ thermally cross-linked and solidified polymer electrolyte with polyethylene glycol diacrylate (PEGDA) as scaffold in which succinonitrile (SN) and lithium bis-trifluoromethanesulfonimide (LiTFSI) were further introduced to improve the ionic conductivity. Herein, the composite gel was served as not only solid-solid interface material but also solid-state electrolyte. Different with conventional polymer gels, the solvent evaporation could not happen for this composite material during the solidification process, and therefore resulting in good interface contact without inside bubbles. We further present the investigation on transport principle of Li+ in the solid-state electrolyte and the effect of molecular chain on ionic conductivity. The conductivity of the solid-state electrolyte can reach 1.76 × 10−4 S cm−1 at room temperature without any assistance of liquid electrolytes, which is attributed to the short molecular chain of PEGDA. Electrochemical window of the solid-state electrolyte can reach 5.2 V after cross-linking treatment. And the lithium-oxygen battery using this solid-state electrolyte can stably cycle for more than 1100 cycles with a current density of 200 mA g−1 and a limit capacity of 200 mAh g−1 at room temperature.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Deyu Mao,Shenglong Yi,Zirui He,Qiancheng Zhu
Lithium-oxygen (Li-O 2 ) batteries with high theoretical energy density are well developed over the past decade, as the cycle performance and round-trip efficiency had enhanced prominently. However, there are still several obstacles that need to be tackled before commercial application. Among them, proper cathode structure design with low cost stands as a core problem. A Typical type of gas diffusion layer cathode are usually carbon paper, which is valuableness, meanwhile, cannot fit the application of flexible devices. In this work, non-woven fabrics were applied as basis materials to synthesis Fe 3 C/N-doped carbon tubes gas diffusion layer by a simple carbonization method. The resulting carbon cloth can be used directly as binder-free and current collector-free cathode for Li-O 2 batteries. More than 130 stable cycles were achieved. The composite synthesized in this paper has the possibility for future application in flexible lithium-oxygen batteries and provide a new strategy for the recovery of non-woven fabrics.
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Advanced Energy Materials
·
2022
·Vol. 12
·期 12
·2102764
·
IF 29.698
Zongqiang Sun,Xiaodong Lin,Wenjie Dou,Yanyan Tan,Ajuan Hu,Qing Hou,Ruming Yuan,Mingsen Zheng,Quanfeng Dong
The large charge overpotential and poor cycling stability triggered by sluggish Li 2 O 2 oxidation kinetics and severe superoxide-related side reactions greatly restrict the development and application of lithium–oxygen batteries. Finding out high-efficiency catalysts that can effectively facilitate a highly reversible formation/decomposition of lithium peroxide is still a crucial challenge in the field of Li–O 2 batteries. Herein, a soluble catalyst of 2,2'-Azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) diammonium salt (ABTS) that can promote highly reversible formation and decomposition of Li 2 O 2 during discharge and charge processes is reported for the first time. During discharge, it can capture and couple two LiO 2 intermediates via its sulfonate and ammonium ions, and induce the intramolecular disproportionation reaction to produce Li 2 O 2 through ionic microenvironment, which not only prompts the solution-phase growth of Li 2 O 2 , but also restricts the reactivity of LiO 2 intermediate, thus significantly alleviating the electrode surface passivation issue and suppressing the superoxide-related side reactions. During charge, it can quickly transport electrons between the electrode and Li 2 O 2 by serving as a new kind of redox mediator (RM), thus greatly facilitating the Li 2 O 2 oxidation kinetics. As a result, the Li–O 2 batteries that incorporate ABTS exhibit outstanding electrochemical performance, low charge overpotential, high discharge capacity, and high cycling stability.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Shaolong Wang,Dingding Ye,Hao Liu,Xun Zhu,Zhenfei Liu,Rong Chen,Qiang Liao,Yang Yang
The in-situ H 2 O 2 electrosynthesis by two-electron oxygen reduction reaction employing renewable electricity is a promising alternative to traditional anthraquinone process due to its security, environmental friendliness and excellent cost effectiveness, which requires high-performance, cost-effective and environmental-friendly electrocatalysts . A bamboo-derived O-doped rocky electrocatalyst is developed by facile pyrolysis and acid treatment for high-efficiency electroreduction of O 2 to H 2 O 2 . Three-dimensional interconnected hierarchical pores in rocky electrocatalysts expose abundant electroactive sites and facilitate mass transfer of reaction species. From the results of rotating ring-disk electrode test, a H 2 O 2 selectivity up to 80% and superior electrocatalytic activity of the prepared electrocatalyst are achieved by surface oxygen functionalization induced by acid treatment. At the optimal catalyst loading of 2 mg cm −2 , prominent H 2 O 2 productivity of 1037 mmol g c a t a l y s t − 1 h − 1 with high current efficiency up to 74.1% is achieved at 30 mA cm −2 by air-breathing cathode. Higher H 2 O 2 productivity (1525 mmol g c a t a l y s t − 1 h − 1 ) is yielded by further raising the current density to 50 mA cm −2 . Moreover, the durability test of the cathode through ten consecutive runs demonstrates its great stability for electrocatalytic generation of H 2 O 2 . This work inspires the development of promising biomass-derived electrocatalysts for green and sustainable on-site H 2 O 2 electrosynthesis.
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JOURNAL OF NANOBIOTECHNOLOGY
·
2021
·Vol. 19
·期 1
·1-14
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IF 10.435
Zhang Tian,Zheng Qiang,Fu Yike,Xie Congkun,Fan Gonglin,Wang Yifan,Wu Yongjun,Cai Xiujun,Han Gaorong,Li Xiang
Sonodynamic therapy (SDT), presenting spatial and temporal control of ROS generation triggered by ultrasound field, has attracted considerable attention in tumor treatment. However, its therapeutic efficacy is severely hindered by the intrinsic hypoxia of solid tumor and the lack of smart design in material band structure. Here in study, fine α-Fe 2 O 3 nanoparticles armored with Pt nanocrystals (α-Fe 2 O 3 @Pt) was investigated as an alternative SDT agent with ingenious bandgap and structural design. The Schottky barrier, due to its unique heterostructure, suppresses the recombination of sono-induced electrons and holes, enabling superior ROS generation. More importantly, the composite nanoparticles may effectively trigger a reoxygenation phenomenon to supply sufficient content of oxygen, favoring the ROS induction under the hypoxic condition and its extra role played for ultrasound imaging. In consequence, α-Fe 2 O 3 @Pt appears to enable effective tumor inhibition with imaging guidance, both in vitro and in vivo. This study has therefore demonstrated a highly potential platform for ultrasound-driven tumor theranostic, which may spark a series of further explorations in therapeutic systems with more rational material design. Graphical Abstract
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