APPLIED SURFACE SCIENCE
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2023
·
IF 6.7
Xueqing Jin,Yeting Zhang,Jialing Huang,Longyi Xu,Qi Shen,Chunyan Sun
Activation of carbon-halogen bonds is vital for realizing the degradation of halogenated pollutants. Herein, zinc indium sulfides Zn x In 2 S x+3 (x = 1, 2 and 3) with different sulfur vacancies concentration were constructed to achieve photocatalytic decabromodiphenyl ether (BDE209) debromination. Under irradiation, ZnIn 2 S 4 had the most outstanding degradation ability to BDE209, attributing to its abundant surface sulfur vacancies. The sulfur vacancies not only can narrow the forbidden band to increase light absorption and utilization, but more importantly, serve as active sites for the adsorption and activation of C-Br of BDE209. Interestingly, the removal of the first bromine atom from BDE209 on sulfur vacancies behaved as a meta- selective debromination process. The selectivity of meta- debromination is as high as 70%, superior to that on oxygen vacancies enriched photocatalyst. It can be ascribed to the larger vacancy space of sulfur to better accommodate bromine atoms in BDE209, which helps to stabilize the meta- bromine adsorption configuration of BDE209 on sulfur vacancies. Meanwhile, the intermediate configuration is further stabilized under the assistance of the S…Br halogen bond by surrounding sulfur atom at the catalytic interface. This work sheds light on the great potential of larger element vacancies to activate C-halogen bonds in photocatalytic treatment of halogenated pollutants.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 4
·928-935
·
IF 4
Yidan Sun,Fang Liu,Xuerong Wang,Kangkang Lu,Xiaojing Liu,Yan Huang,Fengjiao Yu,Yuhui Chen
Efficient catalysts are highly desirable for the selective electrochemical CO2 reduction reaction (CO2RR). Ni single-atom catalysts are known as promising CO2RR catalysts, while Ni NPs are expected to catalyze the competing HER. In this work, we have modified the Ni NPs by encapsulating them into porous Ni–N–C nanosheets (Ni@Ni–N–C), to boost the synergy between Ni NPs and dispersed Ni–N species towards CO2RR. The CO faradaic efficiency (FECO) reached 96.4% at −0.9 V and retained over 90% in a wide potential window. More importantly, FECO values of over 94% have been obtained from −50 to −170 mA cm−2 with a peak FECO of 99% in a flow cell. Our work demonstrates that the surface modification of Ni NPs can inhibit the unexpected HER and activate the surface sites, offering a practical design strategy for CO2RR catalysts.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Hongxia Chen,Yutian Yang,Rihuang Nie,Cheng Li,Shuangwu Xu,Mengcheng Zhou,Xinyu Zhang,Hongming Zhou
Na 3 V 2 (PO 4 ) 3 has been widely studied due to its stable three-dimensional transmission channel structure as a cathode electrode of sodium ion batteries , but its micro particle size and low intrinsic electronic conductivity limit its further development. Therefore, hierarchical porous micro-nano NVP/C materials were successfully prepared using a metal-organic frameworks (MOFs) precursor. Because of the unique hierarchical porous micro-nano structure, 3D highly conductive network between surface and particles, and high specific surface area, M-NVP/C exhibits outstanding rate capability (95.0 mAh g −1 at a current density of 10 C) and extraordinary stable cycle life (the capacity decays from 111.2 mAh g −1 to 108.8 mAh g −1 after 500 cycles at 1 C, with a capacity retention rate of 97.8 %). This method provides a promising pathway for the application of MOFs in battery materials and promotes the development of SIBs in large-scale energy storage systems.
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JOURNAL OF PHYSICAL CHEMISTRY B
·
2023
·
IF 3.3
Wen Wu,Xia Hu,Zhen Zeng,Di Wu,Hanmei Li,Hui Li
Sorafenib (Sor) is a multitarget kinase inhibitor used clinically to treat hepatocellular carcinoma and renal cancer. In this study, the interaction mechanism of Sor with c-MYC G-quadruplexes (G4) was investigated at the molecular level by computer-aided means and experiments. Molecular docking results predicted the binding of Sor to the groove of G4. Molecular dynamics (MD) simulations were used to evaluate the effect of ligand binding to G4. Ultraviolet (UV), fluorescence spectroscopy, and viscosity experiments showed that the binding site was in the groove. The UV and fluorescence titration results showed that compared with traditional G4 ligands represented by compound meso-tetra (N-methyl-4-pyridyl) porphine (TmPyP4), Sor has a lower affinity for G4. Likewise, results from fluorescence resonance energy transfer (FRET) experiments suggested that Sor could have a limited ability to stabilize G4, but it was not as prominent as that of TmPyP4. Time-resolved fluorescence spectroscopy again supported the results from steady-state fluorescence spectroscopy, indicating that a static quenching mechanism mainly drove the process. Studying the interaction mechanism of Sor and c-MYC may inspire the screening of new, selective c-MYC G4 ligands and provide ideas for the design of drugs with good stability, low toxicity, and specific targeting of G4.
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CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Ping Zhang,Hao Chen,Lin Chen,Ying Xiong,Ziqi Sun,Haoyu Yang,Yingke Fu,Yaping Zhang,Ting Liao,Fei Li
Atomically dispersed catalytic metal sites anchored on N-doped carbon support catalysts (M-N-C) show great prospects for CO 2 electroreduction. Here, single-layer NiZn layered double hydroxides (NiZn-LDHs) was used as a sacrificial assistant to fabricate single-Ni atom anchored on ultrathin porous carbon catalyst. NiZn-LDHs were exfoliated to single-layer by polyhydroxy compounds which took as the carbon resource in Ni-N-C, and single layer NiZn LDHs taking as the Ni resource could avoid the agglomeration of Ni atoms during calcining. The CO Faradaic efficiency (FE CO ) of the synthesized Ni-N-C catalyst exceeded 90% at −0.6 to −1.0 V and a FE CO of 95.2% with a current density of 24 mA cm −2 at −0.9 V. This work not only provides a new method for preparing M-N-C catalysts, but also offers an effective and controllable strategy for large-scale production of high-performance single-atom catalysts.
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RARE METALS
·
2023
·Vol. 42
·期 5
·1516-1525
·
IF 8.8
Wang Mei-Ling,Zhao Jin,Wang Jin-Jin,Zhang Jun-Ming,Tian Yu-Zhu,Yue Zhi-Zhu,Li Dong,Hu Tian-Jun,Jia Jian-Feng,Wu Hai-Shun
metal oxide electronic interactions in composite electrocatalysts have a considerable impact on their catalytic capability. In this study, we successfully synthesized an electrocatalytic material composed of MoO 3 /C species-supported Pd nanoparticles (Pd-MoO 3 /C) using a convenient hydrothermal method, which exhibited excellent catalytic activities for both ethanol oxidation and oxygen reduction in KOH media. The specific activity of Pd-MoO 3 /C toward ethanol oxidation with MoO 3 loading (40 wt%) was ~ 2.6 times greater than that for the commercial Pd/C (10 wt%) with the same Pd content. In particular, the activity could effectively hold up to ~ 60% of its maximum activity after 500-cycle tests, demonstrating improved cyclical stability. Notably, the fast electron transfer kinetics toward oxygen reduction for Pd-MoO 3 /C (40%) were also comparable to those of commercial Pt/C (20 wt%) catalysts. These superior electrochemical features are primarily derived from the stronger electronic coupling between Pd and MoO 3 through charge transfer, which can supply more active centers and improve the anti-poisoning ability. Meanwhile, the MoO 3 species in the Pd-MoO 3 /C composite may provide additional benefits in terms of electrical conductivity and dispersion. Graphical Abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Zhao Du,Huayi Cai,Zhiyuan Zhao,Zhonglu Guo,Jing Lin,Yang Huang,Chengchun Tang,Guifeng Chen,Yi Fang
Herein, the graphene quantum dots (GQDs) as a photosensitizer have been introduced on the surface of C-doping porous BN nanoribbons (C-BNNR) to form a series of 0D/1D GQDs/C-BNNR heterojunctions as metal-free catalysts with excellent photocatalytic activity. the C-BNNR with sensitization of GQDs is innovatively applied to the field of CO 2 photocatalytic reduction. The results reveal that GQDs/C-BNNR heterojunctions exhibit excellent optical properties and photocatalytic activity. The CO production rate of GQDs/C-BNNR-3 (33.47 μmol g -1 h -1 ) is 14.49, 4.60 and 2.95 times higher than GQDs (2.31 μmol g -1 h -1 ), BNNR (7.27 μmol g -1 h -1 ) and C-BNNR (11.34 μmol g -1 h -1 ), respectively. This work demonstrates that the addition of GQDs can significantly improve the light utilization of C-BNNR without any effect on the structure. In addition, the strong interaction between the GQDs and C-BNNR leads to the formation of a built-in electric field. It allows photogenerated electrons in GQDs to be transferred into C-BNNR and complexed with holes. As a result, the photogenerated electrons in C-BNNR are induced to participate in the CO 2 photocatalytic reduction process. Meanwhile, GQDs/C-BNNR possess certain CO 2 photocatalytic reduction ability in the NIR region due to the upconversion ability of GQDs. This work pioneer the application of GQDs/C-BNNR heterojunctions in CO 2 photocatalytic reduction and further provides new ideas for the design of novel metal-free catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Ke Zhang,Yajing Wei,Hongyang Cao,Yue Xin,Chuanyi Wang
Tuning reactive oxygen species in peroxymonosulfate (PMS) activation by the structure of catalysts has been extensively studied. But in photocatalysis , the photothermal effect is lack of attention on the alteration of reactive species produced by PMS activation. In this work, ZnFe 2 O 4 /C photocatalyst with oxygen vacancy (ZFO v /C) was synthesized via the calcination of bimetallic Zn/Fe-metal–organic framework. The photocatalytic performance of the catalyst had been studied under several conditions, and the experimental results demonstrated that the photocatalytic reaction rate constant of ZFO v /C photocatalyst without temperature control was 21.3 % higher than that under temperature control. Reactive species quenching experiments and electron paramagnetic resonance indicated that 1 O 2 and h + are the primary reactive species without temperature control, while only 1 O 2 are the dominant reactive species under temperature control conditions. The possible activation site was speculated by in-situ Raman spectroscopy , XPS spectra and cycling experiment. This paper analyzes the reasons for photocatalysis to improve the degradation rate of pollutant from the perspective of the change of reactive species generated by photothermal effect on PMS activation, which may open up opportunities to explore the maximum utilization of sunlight in PMS activation.
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Journal of Energy Storage
·
2023
·
IF 9.4
Xin Xu,Shang Wu,Yang Liu,Chaoyang Liu,Xin Sun,Shuo Tian,Lan Wu,Yuzhi Sun,Zhichao Wang,Quanlu Yang
The tubular microsphere structure is an effective structure for asymmetric supercapacitors due to its high specific surface area and porosity. It can slow down the volume shrinkage caused by redox process. In this paper, tubular-like NiMoO 4 ·xH 2 O microspheres were designed to reach a high specific capacity. The NiMoO 4 ·xH 2 O was prepared by hydrothermal method and subsequent annealing treatment showed a tubular microsphere structure with many particles uniformly distributed. And its specific capacity is 943 F g −1 at 1 A·g −1 and capacity retention is 73.4 % after 3000 cycles. The Bi 2 S 3 /C was selected as negative material to build an asymmetric supercapacitor (battery-type device). It exhibited an impressive specific capacity (419 F g −1 at 1 A g −1 ). It was worth noting that the battery-type devices built with NiMoO 4 ·xH 2 O and Bi 2 S 3 /C can achieve a specific energy of 27.1 Wh kg −1 at 2456.9 W kg −1 and capacity retention of 69.2 % after 5000 cycles. It was shown that NiMoO 4 -xH 2 O and Bi 2 S 3 /C as electrode materials have great potential and can enhance the energy storage application of supercapacitors.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Jun Li,Liying Cai,Xiaosi Liang,Shuke Huang,Xiaosha Wang,Yongshuai Kang,Yongjian Zhao,Lei Zhang,Chenyang Zhao
Light-metalloid-atom-doped Pd interstitial nanoalloy is promising candidate for electrocatalysis because of the favorable electronic effect. Herein, an innovative method was developed to synthesize C-doped Pd interstitial nanoalloy using palladium acetate both as metal precursor and C dopant. Elaborate characterizations demonstrated that C atoms were successfully doped into the Pd lattice via self-catalytic decomposition of acetate ions. The as-synthesized C-doped Pd catalysts showed excellent activity and durable stability for formic acid electrooxidation. The mass activity and specific activity at 0.6 V of C-doped Pd were approximately 2.59 A/mg and 3.50 mA cm −2 , i.e., 2.4 and 2.6 times of Pd, respectively. DFT calculations revealed that interstitial doping with C atoms induced differentiation of Pd sites. The strong noncovalent interaction between the Pd sites and the key intermediates endowed Pd with high-selectivity to direct routes and enhanced CO tolerance. This work presents a sites-differentiation strategy for metallic catalysts to improve the electrocatalysis.
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BIOTECHNOLOGY AND BIOENGINEERING
·
2023
·Vol. 120
·期 5
·1346-1356
·
IF 3.8
Jia-Qi Liu,Xin Ma,Dong-Feng Liu,Chuan-Wang Yang,Dao-Bo Li,Di Min,Han-Qing Yu
Dissimilatory metal-reducing bacteria (DMRB) can transfer electrons to extracellular insoluble electron acceptors and play important roles in geochemical cycling, biocorrosion, environmental remediation, and bioenergy generation. c -type cytochromes ( c -Cyts) are synthesized by DMRB and usually transported to the cell surface to form modularized electron transport conduits through protein assembly, while some of them are released as extracellularly free-moving electron carriers in growth to promote electron transport. However, the type of these released c -Cyts, the timing of their release, and the functions they perform have not been unrevealed yet. In this work, after characterizing the types of c -Cyts released by Geobacter sulfurreducens under a variety of cultivation conditions, we found that these c -Cyts accumulated up to micromolar concentrations in the surrounding medium and conserved their chemical activities. Further studies demonstrated that the presence of c -Cyts accelerated the process of microbial extracellular electron transfer and mediated long-distance electron transfer. In particular, the presence of c -Cyts promoted the microbial respiration and affected the physiological state of the microbial community. In addition, c -Cyts were observed to be adsorbed on the surface of insoluble electron acceptors and modify electron acceptors. These results reveal the overlooked multiple roles of the released c -Cyts in acting as public goods, delivering electrons, modifying electron acceptors, and even regulating bacterial community structure in natural and artificial environments.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Yang Yu,Xiaoping Cai,Xinyang Jiao,Chengyi Xu,Jinan Niu,Peizhong Feng
Ni-Al-Cr intermetallic compounds are candidate at extreme environment due to their excellent oxidation resistance at high temperature, and the oxidation resistance of Ni-Al-Cr alloy system has been studied extensively. However, the research on oxidation resistance mechanism of porous Ni-Al-Cr intermetallic compounds is still not deep. In our work, porous Ni-Al-Cr intermetallic compounds were synthesized by thermal explosion, and the oxidation resistance of porous Ni-Al-Cr system was mainly investigated. The results indicate that Cr promotes the formation of highly protective continuous Al 2 O 3 layer, increasing the oxidation resistance at 900 °C of porous Ni-Al-Cr. After oxidation at 900 °C for 120 h, the minimum mass gain of Ni-Al-Cr products is only 6.96%.
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