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- A novel ternary Z-scheme g-C3N4/CQDs/FeVO4 heterojunction for photodegradation of levofloxacin via peroxymonosulfate activationPublication . Li, Yunuo; Han, Pengda; Zhang, Dongzhe; Zhang, Wenzhi; Chai, Dong-feng; Meng, Lijian; Meng, Lijian; Liming, Bai; Zhao, Ming; Dong, GuohuaCurrently, it is still a significant challenge for photodegradation of the emerging pollutants using g-C3N4 (CN) due to their interior visible light responsibility and rapid recombination of e-/h+. Herein, a novel Z-scheme g-C3N4/CQDs/FeVO4 (CCF) photocatalyst was synthesized by initially preparing hollow tubular g-C3N4/CQDs (CC) and then anchoring FeVO4 on CC. The morphology, structural composition and photoelectrochemical performance of the CCF were investigated by comprehensive characterization such as FT-IR, XPS, XRD, SEM and photoelectrochemical performance tests. The CCF shows superior photodegradation capability toward LFX via activation of peroxymonosulfate (PMS), resulting in a photodegradation efficiency ∼ 97.3 % in the optimal conditions. Apart from the strengthened light responsibility, improved BET specific surface area and porous texture of CCF, the improved photodegradation properties can be ascribed to the formed Z-scheme heterojunction between CC and FeVO4, which can ameliorate the separation efficiency of e-/h+ and accelerate their transfer rate. The addition of CQDs can also serve as a channel for promoting the rapid transfer of photogenerated e-/h+. The photodegradation processes of LFX including generation of reactive oxygen species (ROS) and removal pathways were systematically explored by using radical capturing assays, electron spin resonance (ESR) tests and liquid chromatography-mass spectrometry (LC-MS) techniques. To sum up, this study provides an innovative method for regulating the photocatalytic activity of g-C3N4 via constructing Z-scheme heterostructures and incorporating CQD to degrade emerging contaminants.
- Multimetallic layered double hydroxides as efficient and durable oxygen evolution catalysts for anion exchange membrane water electrolysis at high current densitiesPublication . Yaowen Xu, Kaiyang Xu, Hao Tan, Haoliang Huang, Fei Lin, Chenyue Zhang, Jingwei Wang, Run Ran, Jinfeng Zeng, Zhipeng Yu, Sitaramanjaneya Mouli Thalluri, Lijian Meng, Dehua Xiong and Lifeng Liu
- Confined RuP2 Nanoparticles in N,P,S-tridoped Carbon as Superior Electrocatalyst for pH-Wide Hydrogen EvolutionPublication . Yu Sun, Haibo Li, Suyuan Zeng, Rui Li, Qingxia Yao, Hongyan Chen, Yinghua Wang, Konggang Qu, Lijian Meng
- Ultrafine Ru on Reduced Graphene Oxide-La2O3 Binary Support for Highly Efficient Hydrogen Evolution ReactionPublication . iaying Zhang; Qijing Zhang; Jingyi Qiu; Xiaoying Zhang; Zhiyuan Zhu; Hongyan Chen; Konggang Qu; Lijian Meng
- A novel ternary Z-scheme g-C3N4/CQDs/FeVO4 heterojunction for photodegradation of levofloxacin via peroxymonosulfate activationPublication . Yunuo Li, Pengda Han, Dongzhe Zhang, Wenzhi Zhang, Dong-feng Chai, Lijian Meng, Liming Bai, Ming Zhao, Guohua Dong
- Covalent organic framework assisted low-content ultrafine ru on porous N-doped carbon for efficient hydrogen evolution reactionPublication . Kong-Gang Qu; Zhi-Fei Chen; Li-Hui Wang; Hai-Bo Li; Su-Yuan Zeng; Rui Li; Li-Jian Meng; Hong-Yan Chen; Qing-Xia Yao(Excerpt) Pt-based materials are the benchmarked catalysts in the cathodic hydrogen evolution reaction (HER) of water splitting; the prohibitive cost and scarcity of Pt immensely impede the commercialization of hydrogen energy. Ru has aroused significant concern because of its Pt-like activity and much lower price. However, it’s still a top priority to minimize the Ru loading and pursue the most superior cost performance. Herein, N-rich covalent organic framework (COF) was employed to assist the preparation of ultrafine Ru, including nanoclusters and single atoms loaded onto porous N-doped carbon by a simple impregnation-pyrolysis process with a low Ru content of 6.60 wt%, exhibiting superior HER activity with mass activity of 21.86 and 11.52 A mg-1 Ru (@100 mV) in alkaline and acidic conditions, separately 14.7 and 2.12 times higher than that of commercial Pt/C.
- Microwave-assisted synthesis of hierarchical BiOBr/BiOF Z-scheme heterojunction for activating peroxymonosulfate toward photodegradation of the recalcitrant levofloxacinPublication . Guohua Dong; Dongzhe Zhang; Xinjia Zhang; Zhuangfang Zhang; Dong-feng Chai; Lijian Meng; Jinlong Li; Ming Zhao; Wenzhi ZhangHerein, a novel Z-scheme BiOBr/BiOF heterojunction was synthesized via one-step microwave-assisted hydrothermal method, which was integrated with peroxymonosulfate (PMS) to design a sulfate radical (•SO4−) based advanced oxidation processes (AOPs) system through PMS activation (BiOBr/BiOF-PMS) toward Levofloxacin (LFX) photodegradation. In order to achieving an optimal degradation efficiency, the formed BiOBr/BiOF-PMS was systematically investigated and the operational parameters for LFX photodegradation were thoroughly optimized. Thereby, the optimal BiOBr/BiOF exhibits a higher photodegradation efficiency of 89.8 % toward LFX via PMS activation compared to others including PMS alone, BiOBr, BiOF and BiOBr/BiOF with varied ratios. Furthermore, the BiOBr/BiOF has superior stability for multiple cycles and universal applicability for degrading various contaminants. This can mainly be attributed that the formed heterojunction between BiOBr and BiOF and the enhanced concentration of oxygen vacancies (OVs) of BiOBr/BiOF heterojunction, which can synchronously promote the separation and transmission of the photogenerated charges (e−/h+) and thereby lead to more reactive oxygen species (ROS). As well, the expanded optical responsiveness and increased specific surface area of BiOBr/BiOF are also mainly responsible for the improved photodegradation capability. Free radical capture experiments and ESR technique verify that the •O2− is the primary ROS and •SO4− and •OH play subordinative role. The photodegradation pathways of LFX were unraveled based on the identified intermediates with a liquid-chromatography-mass (LC-MS) technique. Consequently, this study offers a novel route by developing Bi-based heterojunction photocatalyst to activate PMS for refractory antibiotic photodegradation.
- Ir Nanoparticles Synergistically Regulated by B, N Co-Doping in Carbon for pH-Universal Bifunctional Electrocatalysts towards Energy-Efficient Hydrogen ProductionPublication . Huang, Hongli; Meng, Lijian; li, Haibo; Li, Rui; Zeng, Suyuan; Yao, Qingxia; Chen, Hongyan; Qu, Kong-GangThe ultralow-potential hydrazine oxidation reaction (HzOR) can be integrated with hydrogen evolution reaction (HER) to construct the overall hydrazine splitting (OHzS) system, thus realizing energy-saving hydrogen production. Meanwhile, the real electrocatalytic processes normally involve the constantly changed pH and also need to operate under different pH conditions. Therefore, designing advanced pH-universal electrocatalysts with high compatibility for HER and HzOR is of greatly practical significance. Herein, ultrafine Ir nanoparticles embedding in B, N-codoped carbon (Ir/BNC) were facilely synthesized with one Ir-based complex and boric acid by simple mixing and pyrolysis. To reach the current density of 10 mA cm−2, the bifunctional Ir/BNC merely demands the low potentials of −4.8/-6.3/-38.5 mV for HER, 7.5/157.8/330.1 mV for HzOR, and 19/236/358 mV for OHzS in the alkaline, neutral and acidic electrolytes, respectively, all greatly outperforming commercial Pt/C and displaying the huge energy-saving advantage for pH-universal hydrogen generation over the conventional water splitting. Underlyingly, the codoping of abundant B and N heteroatoms with different electronic modulation effects can play synergistical roles to Ir active sites, endowing with the pH-universal multifunctionality as well as the boosted intrinsic unit activity. Additionally, the large surface area, rich pores and highly graphitized carbon also collectively ensure the remarkable apparent performance for bifunctional HER and HzOR. This work supplies a promising strategy for exploiting pH-universal HER and HzOR bifunctional electrocatalysts, greatly potential to the practical energy-efficient hydrogen generation.
- Gold Single Atom Doped Defective Nanoporous Copper Octahedrons for Electrocatalytic Reduction of Carbon Dioxide to EthylenePublication . Zhao, Yang; Wang, Yanan; Yu, Zhipeng; Song, Chao; Wang, Jingwei; Huang, Haoliang; Meng, Lijian; Liu, Miao; Liu, LifengElectrocatalytic CO2 reduction into high-value multicarbon products offers a sustainable approach to closing the anthropogenic carbon cycle and contributing to carbon neutrality, particularly when renewable electricity is used to power the reaction. However, the lack of efficient and durable electrocatalysts with high selectivity for multicarbons severely hinders the practical application of this promising technology. Herein, a nanoporous defective Au1Cu single-atom alloy (DeAu1Cu SAA) catalyst is developed through facile low-temperature thermal reduction in hydrogen and a subsequent dealloying process, which shows high selectivity toward ethylene (C2H4), with a Faradaic efficiency of 52% at the current density of 252 mA cm−2 under a potential of −1.1 V versus reversible hydrogen electrode (RHE). In situ spectroscopy measurements and density functional theory (DFT) calculations reveal that the high C2H4 product selectivity results from the synergistic effect between Au single atoms and defective Cu sites on the surface of catalysts, where Au single atoms promote *CO generation and Cu defects stabilize the key intermediate *OCCO, which altogether enhances C−C coupling kinetics. This work provides important insights into the catalyst design for electrochemical CO2 reduction to multicarbon products.
- Piezo-photocatalysis synergy in γ-GeSe for highly efficient oxygen evolution reactionPublication . Zhang, Tianqi; Zhou, Long; Chen, Guobo; Wei, Songrui; Sun, Rong; Li, Yunping; Meng, Lijian; Zhang, Guanglong; Xia, Shuwei; Wang, Zhongchang; Qiu, MengSolar-driven semiconductor photocatalysts are highly appealing in applications of environmental remediation and energy conversion. However, photocatalytic reactions, particularly oxygen evolution reaction (OER), are often constrained by the swift recombination of electron–hole pairs, thereby resulting in low reaction efficiency. Although it is effective to separate charge carriers by constructing heterojunctions to form built-in electric field, the lattice mismatch and inefficient interlayer charge transfer of heterojunctions in the photocatalysts limit their further development. Here, we propose a new strategy by constructing an internal electric field for OER through an individual piezoelectric two-dimensional material. The results indicate that the piezoelectric effect regulates the electronic structure, reduces bandgap, improves light absorption efficiency, and that the displacement of positive and negative charge centers is the key factor in the enhanced OER. This research indicates the feasibility of combining piezoelectric properties of two-dimensional materials with OER (1.19 eV), providing new insights and guidance for applying the piezoelectric effect in the OER and opening up a way to promote efficient separation of charge carriers.