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NANOTECHNOLOGY · 2021 ·Vol. 32 ·期 17 ·175604 · IF 3.874

Precise control of the ratiometric fluorescence of dual-emissive B/N-doped carbon dots using pH-dependent bonds

Fan Liu,Yuan Jiang,HaiBao Shao,Chunlei Wang,Shuhong Xu,Rong Zhang

Precise control of the structure and bonds of doped carbon dots (CDs) is important, so that their fluorescence can be tuned as desired. Up until now, there has been a lack of effective ways to control the bonds of doped CDs. In this article, we show that the fluorescence of B/N-doped carbon dots (B/N-CDs) can be precisely tuned just by controlling their precursors' pH values. The prepared B/N-CDs exhibit two emission bands, including one emission peak at around 450 nm due to the defect state caused by low sp2 hybridization of carbon atoms, as well as another emission peak at around 360 nm caused by the B-N bond. The results for the ratio of the maximum intensity of the two emission peaks above show a linear relationship. Meanwhile, the role of the pH value of the precursors on the luminescence of B/N-CDs is deeply studied. On the one hand, the pH value affects the bonding process of CDs. N-H bonds tend to form at a low pH value, while more competitive B-N bonds exist at much higher pH value, leading to the pH-dependent intensity of the 360 nm emission band. On the other hand, a high pH value causes higher crystallinity, thus suppressing defect-state fluorescence at 450 nm. The dual effects of pH lead to precisely controlled dual-emission intensities as well as ratiometric fluorescence.

研究领域: 材料科学 · 化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Boron/nitrogen-trapping and regulative electronic states around Ru nanoparticles towards bifunctional hydrogen production

Shaoxian Song,Song Wu,Yating He,Yiwen Zhang,Guangyin Fan,Yan Long,Shuyan Song

Developing a straightforward and general strategy to regulate the surface microenvironment of a carbon matrix enriched with N/B motifs for efficient atomic utilization and electronic state of metal sites in bifunctional hydrogen production via ammonia-borane hydrolysis (ABH) and water electrolysis is a persistent challenge. Herein, we present a simple, green, and universal approach to fabricate B/N co-doped porous carbons using ammonia-borane (AB) as a triple functional agent, eliminating the need for hazardous and explosive functional agents and complicated procedures. The pyrolysis of AB induces the regulation of the surface microenvironment of the carbon matrix, leading to the formation of abundant surface functional groups, defects, and pore structures. This regulation enhances the efficiency of atom utilization and the electronic state of the active component, resulting in improved bifunctional hydrogen evolution. Among the catalysts, B/N co-doped vulcan carbon (Ru/BNC) with 2.1 wt% Ru loading demonstrates the highest performance in catalytic hydrogen production from ABH, achieving an ultrahigh turnover frequency of 1854 min −1 (depending on the dispersion of Ru). Furthermore, this catalyst shows remarkable electrochemical activity for hydrogen evolution in alkaline water electrolysis with a low overpotential of 31 mV at 10 mA cm −2 . The present study provides a simple, green, and universal method to regulate the surface microenvironment of various carbons with B/N modulators, thereby adjusting the atomic utilization and electronic state of active metals for enhanced bifunctional hydrogen evolution.

CAS / MDL: 14898-67-0 13235-36-4
研究领域: 材料科学 · 催化化学 · 能源科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Highly sensitive fluorescence sensor for mercury(II) based on boron- and nitrogen-co-doped graphene quantum dots

Zhenyu Liu,Zunli Mo,Xiaohui Niu,Xing Yang,Yangyang Jiang,Pan Zhao,Nijuan Liu,Ruibin Guo

In this work, we invented a new method to synthesize boron- and nitrogen-co-doped graphene quantum dots (B, N-GQDs). This synthesis method was more reliable, simple, and environmentally friendly than the bottom-up methods reported in the current literature that use citric acid or other organic materials as the carbon source. Instead, B, N-GQDs were synthesized from graphene oxide (GO) by a top-down method. The obtained B, N-GQDs showed a bright blue luminescence under a UV lamp at 365 nm, and the absolute photoluminescence quantum yield (PLQY) was 5.13%. Because mercury(II) ions (Hg 2+ ) are highly toxic and can seriously affect the ecological environment and human health, the detection of low-concentration Hg 2+ and the establishment of rapid, accurate and sensitive methods for detecting Hg 2+ are of great significance to the activities of life, including those of humans. Therefore, using the good luminescence properties of B, N-GQDs, we invented a new type of fluorescence sensor that can detect Hg 2+ . The sensor was very sensitive to Hg 2+ , had a good linear relationship in the concentration range of 0.2–1 μM, and exhibited a minimum limit of detection of 6.4 nM. Furthermore, this approach was successfully applied to the detection of Hg 2+ in real environmental water samples.

研究领域: 环境科学 · 材料科学 · 分析化学
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS · 2023 · IF 4

High-density defect-induced ultrahigh boron and nitrogen doping of iron–copper-functionalized porous carbon nanosheets for enhanced water splitting

Yibin Wang,Lan Xiao,Mian Li,Yingjie Zhang,Tingting Liu

The high cost of precursors and the complexity of synthesis procedures have hindered the widespread use of two-dimensional (2D) porous carbon nanosheets in water splitting. In this study, we successfully developed a low-cost method for the rapid synthesis of three-dimensional (3D) hierarchically porous architectures self-assembled from iron–copper nanoparticles embedded in boron (B)/nitrogen (N)-codoped 2D porous carbon nanosheets (denoted as FeCu@BNPCNS). The optimal FeCu@BNPCNS-900 nanosheet exhibited a large surface area, abundant porous channels, meso/macropores, and carbon edges/defects. Particularly, 10.25 atom% of B/N electrochemically active centers (such as pyridinic-N (including the metal–nitrogen–carbon species), pyrrolic-N, graphitic-N, and BC 3 ) were successfully doped into the optimal FeCu@BNPCNS-900 nanosheets. In an alkaline solution, FeCu@BNPCNS-900 exhibited excellent electrocatalytic activity for hydrogen evolution reaction (HER), which was higher than that of the commercial 20 wt% Pt/C. For example, the HER potential of FeCu@BNPCNS-900 at 10 mA cm −2 [ E 10 ; −202.3 mV vs. reversible hydrogen electrode (RHE)] was only 140.2 mV more negative than that of 20 wt% Pt/C (−62.1 mV vs. RHE). Additionally, FeCu@BNPCNS-900 exhibited a slightly lower oxygen evolution reaction (OER) electrocatalytic activity than the ruthenium oxide (RuO 2 ). Particularly, the OER E 10 potential (+1.634 V vs. RHE) of FeCu@BNPCNS-900 was only 76 mV more positive than that of RuO 2 (+1.558 V vs. RHE). The FeCu@BNPCNS-900||FeCu@BNPCNS-900 cell achieved 10 mA cm −2 at 1.613 V, which was 58 mV more negative than that of the 20 wt% Pt/C||RuO 2 cell (1.671 V). The excellent water-splitting performance of FeCu@BNPCNS-900 could be attributed to the 3D hierarchically porous architecture, abundant channels/mesopores, and uniformly dispersed electrocatalytically active sites. Therefore, we developed an efficient strategy for the large-scale and low-cost synthesis of 2D porous carbon nanosheets without the need for precursors, templates, or surfactants .

研究领域: 材料科学 · 能源化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Palladium nanoparticles supported on flower-like boron, nitrogen doped carbon for electrochemical oxidation ethanol reaction

Yan Su,Caifeng Li,Lijian Xu,Jie Xue,Wenbo Yuan,Chenxue Yao,Jinglei Liu,Mengmeng Cheng,Shifeng Hou

We loaded palladium (Pd) nanoparticles (NPs) onto a flower-like boron (B), nitrogen (N) doped carbon carrier via a cobalt reduction path. The B, N co-doped flower-like carbon carrier itself (BNCF-800) was prepared by the pyrogenation process of flower-like cobalt boronoisophthalic acid (Co-BA), which was produced through the coordination between Co 2+ , derived from the zeolitic imidazolate frameworks (ZIF-67), and 5-boronoisophthalic acid. The abundant activity sites caused by B, N doped carbon are able to anchor the Pd nanoparticles further during the cobalt reduction process to prevent the agglomeration of Pd NPs on the BNCF-800 carrier. The flower-like construct of carbon composites also offers more open spaces and paths to promote mass and charge transmission in the catalyst process. Hence, the palladium catalyst immobilized on the flower-like B, N doped carbon exhibited electro-catalyst performance toward an ethanol oxidation reaction (EOR). The mass activity of the Pd/BNCF-800 was 1989.20 mA mg −1 , which is 2.84 times that of the Pd/C in the basic electrolyte.

CAS / MDL: 881302-73-4
研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Synthesis of three-dimensional (3D) hierarchically porous iron–nickel nanoparticles encapsulated in boron and nitrogen-codoped porous carbon nanosheets for accelerated water splitting

Mian Li,Fei Guo,Lan Xiao,Yibin Wang,Yingjie Zhang,Xiangjie Bo,Tingting Liu

Designing two-dimensional (2D) porous carbon nanosheets is a promising strategy for enhancing the water-splitting activities of non-noble metal catalysts . In this study, we developed a novel method for synthesizing the novel three-dimensional (3D) hierarchically porous iron–nickel (FeNi) nanoparticles encapsulated in boron (B) and nitrogen (N)-codoped porous carbon nanosheets (denoted as FeNi@BNPCNS). Owing to the advantages of morphology and structure of B and N, 10.31 atom % of B/N active centers were successfully doped into the optimal FeNi@BNPCNS-800 nanosheets . FeNi@BNPCNS-800 exhibited better hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) electrocatalytic activities than control catalysts in an alkaline solution. However, the HER and OER electrocatalytic activities of FeNi@BNPCNS-800 were slightly lower than 20 wt% Pt/C and RuO 2 . The FeNi@BNPCNS-800||FeNi@BNPCNS-800 electrolyzer achieved 10 mA cm −2 at 1.514 V, which was 73 mV lower than that of 20 wt% Pt/C||RuO 2 electrolyzer (1.587 V). The perfect 3D honeycomb-like architectures, abundant mesopores/defects, and abundant electrocatalytic active sites were attributed to the outstanding water-splitting performances of FeNi@BNPCNS-800 nanosheets . This study provides an efficient strategy for the large-scale, rapid, and low-cost fabrication of 2D porous carbon nanosheets without using any template, surfactant , or expensive raw material, thus presenting a simple approach to design advanced non-noble metal electrocatalysts for water splitting.

研究领域: 材料科学 · 能源化学
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY · 2020 · IF 4.192

Efficient Imaging of Saccharomyces cerevisiae Based on B- and N-Doped Carbon Dots

Yun Ma,Zhi Ma,Xiyue Huo,Meiyu Gu,Sainan Ma,Yu Jing,Yixiao Wang,Ying Yue,Zhibiao Feng,Bo Tian

The estimation of yeast viability with B- and N-doped carbon dots (BN-CDs) was investigated in this paper. BN-CDs with a fluorescent quantum yield of 65.47% were prepared by a one-step hydrothermal method. The size distribution of BN-CDs was relatively narrow, with the majority falling within 7.5–8.5 nm, and they were mainly composed of carbon, oxygen, nitrogen, and boron. BN-CDs were shown to have strong and stable fluorescence. They exhibited excitation-independent photoluminescence property, which could avoid the autofluorescence and limitation of the excitation source. Dead and live yeast cells were distinguished well by BN-CD staining in a short time, and there was no strict requirement for light protection. The application of BN-CDs in beer brewing can solve the problem of estimation of yeast viability.

研究领域: 微生物学 · 材料科学 · 生物技术
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

Graphitized and curved carbon nanochambers embedded with highly-dispersed cobalt moieties for oxygen reduction electrocatalysis

Caimei He,Danling Zhang,Fengshang Chen,Yezheng Cai,Xiangsi Wu,Zhaoling Ma,Youguo Huang,Kui Liu,Qiang Wu,Hongqiang Wang,Qingyu Li

Designed synthesis of robust while earth-abundant carbon-based electrocatalysts for oxygen reduction reaction (ORR) is central for the wide spread application of renewable energy conversion technologies. Herein, graphitized and curved carbon nanochambers decorated with boron and nitrogen tailored highly-dispersed cobalt moieties (B,N-Co/GCCN) were developed via a feasible strategy combining room temperature crosslinking and in situ catalytic graphitization processes. The graphitized and curved carbon nanochambers enhanced the electron transfer and structural stability and tailored the electronic structure of metal active sites. Moreover, the in situ coupled amorphous carbon and cobalt-nitrogen/boron moieties represented catalytically active sites for catalyzing ORR. Notably, the selected B doping made the electron density of Co of B,N-Co/GCCN higher compared to N-Co/GCCN, promoting the adsorption and activation of oxygen molecule. Benefiting from this integrated structure, the B,N-Co/GHC exhibited high ORR activity comparable to commercial Pt/C catalyst, along with robust electrocatalytic stability with little change in half-wave potential after 5000 cycles. Impressively, a homemade zinc-air battery driven by B,N-Co/GHC showed higher discharging performance than the one driven by Pt/C, demonstrating promising application prospect.

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

B,N-Doped PdRu Aerogels as High-Performance Peroxidase Mimics for Sensitive Detection of Glucose

Yuting Zeng,Yan Li,Xiaofeng Tan,Jindi Gong,Ziyu Wang,Yuhao An,Zhenqiang Wang,He Li

Among plentiful porous nanomaterials, noble metal aerogels taken as nanozymes attract broad attention in sensing applications with their distinct enzyme mimic functions. In the catalytic field, the heteroatom doping strategy is a kind of way with great promise in improving the enzyme mimic activity of noble metal aerogels. In this experiment, we find a type of creative materials that were prepared by the fast and simple method. Due to the unique porous structure and synergetic effect from doped atoms, PdRu aerogels co-doped with boron and nitrogen (B, N-PdRu aerogels) were prepared using NH3BH3 as a reductant, which present improved peroxidase mimicking activity. With the existence of H2O2, the oxidation of 3,3′,5,5′-tetramethylbenzidine was catalyzed by B, N-PdRu aerogels fairly efficiently, whose solution would be a blue appearance at optimum absorption wavelength 652 nm. Thus, by the tandem reaction bound to the enzyme glucose oxidase, the B, N-PdRu aerogels can be used for the sensitive determination of glucose. The new method has a good linear detection effect for glucose in the range of 10 μM to 2 mM. The minimum limit of detection can reach as low as 6 μM. This work will contribute to research on the rational design of metal aerogels based on the heteroatomic doping strategy and enhance the corresponding performance for a variety of applications.

研究领域: 材料科学 · 生物传感 · 催化化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Carboxyl induced ultrahigh defects and boron/nitrogen active centers in cobalt-embedded hierarchically porous carbon nanofibers: The stable oxygen reduction reaction catalysis in acid

Mian Li,Fei Guo,Lan Xiao,Yibin Wang,Yingjie Zhang,Xiangjie Bo,Tingting Liu

Transition metal-nitrogen-carbon (M N C) type catalysts have been considered a promising alternative to noble metals for oxygen reduction reaction (ORR) electrocatalysis. Nevertheless, poor stabilities of M N C catalysts in acidic solutions limit their commercialization. In this study, we design and synthesize novel three-dimensional (3D) cobalt (Co) nanoparticles encapsulated in ultrahigh content of boron (B) and nitrogen (N) -doped hierarchically porous carbon nanofibers (denoted as Co@BN-PCNFs) by carbonizing the 3D acetic acid/cobalt nitrate/4-hydroxybenzeneboronic acid/polyvinylpyrrolidone precursor networks woven using electrospinning method under a nitrogen atmosphere. The optimal Co@BN-PCNFs-900 catalyst has abundant micro/mesopores and numerous topological defects and exhibits the largest surface area. Under the synergistic effect of oxygen-containing acetic acid molecules and the electrospinning technology, 5.87 at.% of B and 5.91 at.% of N atoms were doped into carbon nanofibers. Specifically, B/N electrocatalytic active centers (including BC 3 , pyridinic-N/Co N C, pyrrolic-N, and graphitic-N) of approximately 8.70 at.% were successfully introduced into the skeletons of Co@BN-PCNFs-900. In 0.1 M KOH, the ORR onset potential ( E onset ) and half-wave potential ( E 1/2 ) of Co@BN-PCNFs-900 were ∼ 64 and ∼ 63 mV, respectively, more positive than those of 20 wt% Pt/C. Additionally, in 0.5 M H 2 SO 4 , the ORR E onset and E 1/2 values of Co@BN-PCNFs-900 were only ∼ 11 and ∼ 7 mV, respectively, more negative than those of 20 wt% Pt/C. As the 3D hierarchically porous architectures, topological carbon edges, BC 3 , and partial N C/Co N C are relatively stable, the Co@BN-PCNFs-900 exhibits excellent stability toward ORR catalysis in both acidic and basic media. These favorable properties of Co@BN-PCNFs-900 nanofibers make them the best non-noble metal-based carbonaceous electrocatalysts for ORR in acidic electrolytes.

研究领域: 材料科学 · 电化学 · 催化科学
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2019 ·Vol. 30 ·期 21 ·19119-19125 · IF 2.195

Boron nitride doped Li7P3S11 solid electrolyte with improved interfacial compatibility and application in all-solid-state Li/S battery

Xu Xiaoyan,Wang Lei,Fei Huifang,Ci Lijie

All-solid-state lithium sulfur battery is considered as one of the most promising candidates for the future application due to high theoretical energy density and enhanced safety. However, the all-solid-state lithium sulfur battery based on Li 7 P 3 S 11 solid electrolyte has serious interface issues between electrode and solid electrolyte. The reaction of lithium metal and Li 7 P 3 S 11 solid electrolyte would form a layer without lithium-ion conducting, which could impend the lithium-ion transfer and transport during cycling and causes increase of internal resistance and capacity fading. Herein, we introduce a solid electrolyte Li 7 P 3 S 11 with BN doping for the all-solid-state lithium sulfur battery. The BN nanoflakes could partially isolate the Li 7 P 3 S 11 solid electrolyte and lithium metal, thus improving the interfacial compatibility of electrode and electrolyte. With BN doped Li 7 P 3 S 11 used as solid electrolyte, the all-solid-state Li/S battery exhibits an enhanced electrochemical performance with better cycling stability and higher Coulombic efficiency.

研究领域: 材料科学 · 电化学 · 能源存储
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Flexible all-solid-state supercapacitors based on boron and nitrogen-doped carbon network anchored on carbon fiber cloth

Lei Shi,Junwei Ye,Hao Lu,Guangyao Wang,Jialin Lv,Guiling Ning

The rapid development of wearable electronic devices has created a huge demand for flexible all-solid-state supercapacitors (FSSCs), and high-performance electrode materials for FSSCs are strong desired simultaneously. In this work, boron and nitrogen-doped carbon (BCN) anchored on active carbon fiber cloth (ACC) are specially designed and manufactured by immersing ACC in a mixed solution of urea, boric acid and polyethylene oxide-propylene oxide (P123) and then calcining, which can be used to assemble high-performance FSSCs as electrodes. The three-dimensional (3D) cross-linked network of BCN grown on the carbon fibers improves the transmission rate of electrons and provides abundant electrochemical reaction sites, which are conducive to the performance of supercapacitors. Thanks to this structural advantage, the ACC@BCN electrode exhibits an area specific capacitance of 1018 mF cm −2 and a volume specific capacitance of 535.8 F g −1 at a current of 1 mA cm −2 . Furthermore, the symmetric FSSCs based on ACC@BCN show high energy density of 1.573 mWh cm −3 and power density of 128.7 mW cm −3 , and the capacitance retention can still keep 89.5% even after 10,000 cycles. This work provides a simple and effective way for large-scale preparation of high-performance, high-stability electrode materials for wearable electronic devices.

研究领域: 材料科学 · 能源技术
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