筛选条件 :
Hongbin YANG
Changhong Wang; Zhengyang Liu; Quanxiao Peng; Dandan Xing; Tao Hu; Feng Du
Angewandte Chemie,
2025
137
(3)
摘要 : Electrochemical reduction of nitrate to ammonia (NRA) offers a sustainable approach for NH3 production and NO3− removal but suffers from low NH3 yield rate (<1.20 mmol h−1 cm−2). We present bimetallic Cu11Ag3 nanotips with tailored local environment, which achieve an ultrahigh NH3 yield rate of 2.36 mmol h−1 cm−2 at a low applied potential of −0.33 V vs. RHE, a high Faradaic efficiency (FE) of 98.8 %, and long-term operation stability at 1800 mg-N L−1 NO3−, outperforming most of the recently reported catalysts. At a NO3− concentration as low as 15 mg-N L−1, it still delivers a high FE of 86.9 % and an NH3 selectivity of 93.8 %. Finite-element method and density functional theory calculations reveal that the Cu11Ag3 exhibits reduced adsorption energy barrier of N intermediates, favorable water dissociation for H generation and high energy barrier for H2 formation, while its tip-enhanced enrichment promoting NO3− accumulation.
Changhong Wang; Zhengyang Liu; Quanxiao Peng; Dandan Xing; Tao Hu; Feng Du
Angewandte Chemie (International ed. Internet),
2025
64
(3)
-
EI
SCIE
摘要 : Electrochemical reduction of nitrate to ammonia (NRA) offers a sustainable approach for NH3 production and NO3− removal but suffers from low NH3 yield rate (<1.20 mmol h−1 cm−2). We present bimetallic Cu11Ag3 nanotips with tailored local environment, which achieve an ultrahigh NH3 yield rate of 2.36 mmol h−1 cm−2 at a low applied potential of −0.33 V vs. RHE, a high Faradaic efficiency (FE) of 98.8 %, and long-term operation stability at 1800 mg-N L−1 NO3−, outperforming most of the recently reported catalysts. At a NO3− concentration as low as 15 mg-N L−1, it still delivers a high FE of 86.9 % and an NH3 selectivity of 93.8 %. Finite-element method and density functional theory calculations reveal that the Cu11Ag3 exhibits reduced adsorption energy barrier of N intermediates, favorable water dissociation for H generation and high energy barrier for H2 formation, while its tip-enhanced enrichment promoting NO3− accumulation.
Lingyue Liu; Jinjie Liu; Guangchao Li; Xiuwen Shi; Jun Yin; Shourong Zheng
Angewandte Chemie (International ed. Internet),
2025
-1
-
EI
SCIE
摘要 : The thermocatalytic hydrogenation of CO2 to ethanol has attracted significant interest because ethanol offers ease of transport and substantial value in chemical synthesis. Here, we present a state-of-the-art catalyst for the CO2 hydrogenation to ethanol achieved by precisely depositing single-atom Ir species on P cluster islands situated on the In2O3 nanosheets. The Ir1-Px/In2O3 catalyst achieves an impressive ethanol yield of 3.33 mmol g-1 h-1 and a turnover frequency (TOF) of 914 h-1 under 1.0 MPa (H2/CO2 = 3:1) at 180 °C, nearly 8 times higher than that of the unmodified Ir1/In2O3 catalyst. Additionally, at a more industrially relevant pressure of 5.0 MPa, the TOF of the Ir1-Px/In2O3 catalyst can reach up to 2108 h-1, surpassing previously reported catalysts. Combined in-situ characterization and theoretical studies reveal that the hydrogenation process is significantly enhanced by the Ir1-Px entities. Specifically, the Ir atom facilitates CO2 activation and C-C coupling, while the surrounding P island exhibits exceptional H2 dissociation ability. These three steps have been found crucial for the CO2 hydrogenation reaction. This discovery opens new opportunities for the regulation of the microenvironment of current catalysts by providing essential chemical functionalities that enhance intricate and complex reaction processes.
Jincheng Zhang; Fuhua Li; Wei Liu; Qilun Wang; Xuning Li; Sung-Fu Hung
Angewandte Chemie (International ed. Internet),
2024
63
(51)
-
EI
SCIE
摘要 : Single atom catalysts (SACs) are promising non-precious catalysts for oxygen reduction reaction (ORR). Unfortunately, the ORR SACs usually suffer from unsatisfactory activity and in particular poor stability. Herein, we report atomically dispersed manganese (Mn) embedded on nitrogen and sulfur co-doped graphene as an efficient and robust electrocatalyst for ORR in alkaline electrolyte, realizing a half-wave potential (E1/2) of 0.883 V vs. reversible hydrogen electrode (RHE) with negligible activity degradation after 40, 000 cyclic voltammetry (CV) cycles in 0.1 M KOH. Introducing sulfur (S) to form Mn−S coordination changes the spin state of single Mn atom from high-spin to low-spin, verified by electron paramagnetic resonance (EPR) and magnetic susceptibility measurements as well as density functional theory (DFT) calculations, which effectively optimizes the oxygen intermediates adsorption over the single Mn atomic sites and thus greatly improves the ORR activity.
Jincheng Zhang; Fuhua Li; Wei Liu; Qilun Wang; Xuning Li; Sung-Fu Hung
Angewandte Chemie,
2024
136
(51)
摘要 : Single atom catalysts (SACs) are promising non-precious catalysts for oxygen reduction reaction (ORR). Unfortunately, the ORR SACs usually suffer from unsatisfactory activity and in particular poor stability. Herein, we report atomically dispersed manganese (Mn) embedded on nitrogen and sulfur co-doped graphene as an efficient and robust electrocatalyst for ORR in alkaline electrolyte, realizing a half-wave potential (E1/2) of 0.883 V vs. reversible hydrogen electrode (RHE) with negligible activity degradation after 40, 000 cyclic voltammetry (CV) cycles in 0.1 M KOH. Introducing sulfur (S) to form Mn−S coordination changes the spin state of single Mn atom from high-spin to low-spin, verified by electron paramagnetic resonance (EPR) and magnetic susceptibility measurements as well as density functional theory (DFT) calculations, which effectively optimizes the oxygen intermediates adsorption over the single Mn atomic sites and thus greatly improves the ORR activity.
Qiang Zhang; Huinan Che; Hongbin Yang; Bin Liu; Yanhui Ao
Angewandte Chemie (International ed. Internet),
2024
63
(38)
-
EI
SCIE
摘要 : Proton supply is as critical as O2 activation for artificial photosynthesis of hydrogen peroxide (H2O2) via two-electron oxygen reduction reaction (2e− ORR). However, proton release via water dissociation is frequently hindered because of the sluggish water oxidation reaction (WOR), extremely limiting the efficiency of photocatalytic H2O2 production. To tackle this challenge, carboxyl-enriched supramolecular polymer (perylene tetracarboxylic acid—PTCA) is elaborately prepared by molecular self-assembly for overall photosynthesis of H2O2. Interestingly, the interconversion between carboxyl as Brønsted acid and its conjugated base realizes rapid proton circulation. Through this efficient tandem proton transfer process, the spatial effect of photocatalytic reduction and oxidation reaction is greatly enhanced with reduced reaction barrier. This significantly facilitates 2e− photocatalytic ORR to synthesize H2O2 and in the meanwhile promotes 4e− photocatalytic WOR to evolve O2. Consequently, the as-developed PTCA exhibits a remarkable H2O2 yield of 185.6 μM h−1 in pure water and air atmosphere under visible light illumination. More impressively, an appreciable H2O2 yield of 78.6 μM h−1 can be well maintained in an anaerobic system owing to in situ O2 generation by 4e− photocatalytic WOR. Our study presents a novel concept for artificial photosynthesis of H2O2 via constructing efficient proton transfer pathway to enable rapid proton circulation.
Yuanxin Mao; Qing Mao; Hongbin Yang; Qi Liu; Xufeng Dong; Yifan Li
Angewandte Chemie (International ed. Internet),
2024
63
(49)
-
EI
SCIE
摘要 : Oxide derived catalyst displays outstanding catalytic activity and selectivity in electrochemical carbon dioxide reduction reaction (CO2RR), in which, it is found that residue oxygen atoms play a pivotal role in regulating the catalyst's electronic structure and thus the CO2RR process. Unfortunately, the intrinsic thermodynamic instability of oxygen atoms in oxide derived catalyst under cathodic CO2RR potentials makes it unstable during continuous electrolysis, greatly hindering its practical industrial applications. In this work, we develop a pulsed-bias technique that is able to dynamically stabilize the residue oxygen atoms in oxide derived catalyst during electrochemical CO2RR. As a result, the oxide derived catalyst under pulsed bias exhibits super catalytic stability in catalyzing electrochemical CO2RR, while keeping excellent catalytic activity and selectivity.
Xinyi Zou; Mengjie Ma; Changhong Wang; Jingsha Li; Hongbin Yang; Tian C. Zhang
ACS ES&T Water,
2024
4
(7)
-
ESCI
摘要 : In recent years, it has been difficult to remove excess N (mainly NO3–-N) in wastewater with a low ratio of biochemical oxygen demand/chemical oxygen demand. The present study combined the operation of electrochemical process (with a modified brass mesh electrode being used as the cathode) and anammox (anaerobic ammonium oxidation) to treat a high nitrate-simulated wastewater and investigated the overall operating parameters of the combined system. Results showed that the efficiency of the combined system for the removal of total nitrogen can be stabilized over 76.35% at an electrochemical feed of 300 mg/L NO3–-N, and the NO2–-N/NH4+-N (around 130 mg/L) in the effluent of the electrochemical part was kept around 1. Although specific anammox activity decreased from 142.07 to 129.23 mg/g VSS-d, the amount of secreted extracellular polymeric substances increased from an initial 152.10 to 204.12 mg/g VSS. The main functional bacteria were Candidatus Brocadia (2.80–8.84%) and Candidatus Jettenia (0.94–1.99%). Compared to traditional denitrification, the composite process lags behind but still holds a certain economic advantage over electrochemical nitrate removal counterpart.
Yu Gu; Cunxia Fan; Hongbin Yang; Huiping Sun; Xiaobao Wang; Xingchen Qiu
Advanced Biology,
2024
8
(4)
-
EI
SCIE
摘要 : DNA methyltransferase is significant in cellular activities and gene expression, and its aberrant expression is closely linked to various cancers during initiation and progression. Currently, there is a great demand for reliable and label-free techniques for DNA methyltransferase evaluation in tumor diagnosis and cancer therapy. Herein, a low-background fluorescent RNA aptamer-based sensing approach for label-free quantification of cytosine-guanine (CpG) dinucleotides methyltransferase (M.SssI) is reported. The fluorogenic light-up RNA aptamers-based strategy exhibits high selectivity via restriction endonuclease, padlock-based recognition, and RNA transcription. By combining rolling circle amplification (RCA), and RNA transcription with fluorescence response of RNA aptamers of Spinach-dye compound, the proposed platform exhibited efficiently ultrahigh sensitivity toward M.SssI. Eventually, the detection can be achieved in a linear range of 0.02–100 U mL−1 with a detection limit of 1.6 × 10−3 U mL−1. Owing to these superior features, the method is further applied in serum samples spiked M.SssI, which delivers a recovery ranging from 92.0 to 107.0% and a relative standard deviation <7.0%, providing a promising and practical tool for determining M.SssI in complex biological matrices.
Junjie Zhong; Zhanhao Liang; Ning Liu; Yucui Xiang; Bo Yan; Fangyuan Zhu
ACS Nano.,
2024
18
(7)
-
EI
SCIE
摘要 : Unraveling the configuration–activity relationship and synergistic enhancement mechanism (such as real active center, electron spin-state, and d-orbital energy level) for triatomic catalysts, as well as their intrinsically bifunctional oxygen electrocatalysis, is a great challenge. Here we present a triatomic catalyst (TAC) with a trinuclear active structure that displays extraordinary oxygen electrocatalysis for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), greatly outperforming the counterpart of single-atom and diatomic catalysts. The aqueous Zn-air battery (ZAB) equipped with a TAC-based cathode exhibits extraordinary rechargeable stability and ultrarobust cycling performance (1970 h/3940 cycles at 2 mA cm–2, 125 h/250 cycles at 10 mA cm–2 with negligible voltage decay), and the quasi-solid-state ZAB displays outstanding rechargeability and low-temperature adaptability (300 h/1800 cycles at 2 mA cm–2 at −60 °C), outperforming other state-of-the-art ZABs. The experimental and theoretical analyses reveal the symmetry-breaking CoN4 configuration under incorporation of neighboring metal atoms (Fe and Cu), which leads to d-orbital modulation, a low-shift d band center, weakened binding strength to the oxygen intermediates, and decreased energy barrier for bifunctional oxygen electrocatalysis. This rational tricoordination design as well as an in-depth mechanism analysis indicate that hetero-TACs can be promisingly applied in various electrocatalysis applications.