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| Open AccessElectrochemical nitrate reduction in acid enables high-efficiency ammonia synthesis and high-voltage pollutes-based fuel cells
Research on electrochemical nitrate reduction to ammonia in acidic conditions has been less extensive than that conducted in alkaline conditions. Here, the authors report a hybrid of iron phthalocyanine and TiO2 catalyst with improved efficiency toward acidic nitrate reduction and its application in Zn-nitrate batteries and high-voltage pollutes-based fuel cell.
- Rong Zhang
- , Chuan Li
- & Chunyi Zhi
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Article
| Open AccessSynthesizing evidence for the external cycling of NOx in high- to low-NOx atmospheres
External cycling regenerates nitrogen oxides from the NOx oxidative reservoir, NOz. Aircraft observations reveal NOx external cycling compensates for NOx aging, sustaining NOx distribution and production of OH radicals far from NOx emission sources
- Chunxiang Ye
- , Xianliang Zhou
- & Shaojie Song
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Article
| Open AccessThermoelectric coupling effect in BNT-BZT-xGaN pyroelectric ceramics for low-grade temperature-driven energy harvesting
Pyroelectric energy harvesting has received increasing attention due to its ability to convert low-grade waste heat into electricity. Here, authors report an enhanced thermoelectric coupling BNT-BZT-xGaN pyroelectric energy harvester by facilitating resonance vibration between Ga and Ti, O atoms.
- Meng Shen
- , Kun Liu
- & Kui Yao
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Article
| Open AccessA polymer tethering strategy to achieve high metal loading on catalysts for Fenton reactions
This work reports a self-polymerization confinement strategy to develop and synthesize carbon-supported metal catalysts with high metal loading. Efficient Fenton reactivity is observed for samples containing well dispersed iron sites.
- Lixin Wang
- , Longjun Rao
- & Mingyang Xing
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Article
| Open AccessClimate warming and elevated CO2 alter peatland soil carbon sources and stability
No inherently stable peat soil carbon. Researchers found that all molecular components of peatland soil organic carbon responded to warming and eCO2, including the components presumed to be slow cycling and stable.
- Nicholas O. E. Ofiti
- , Michael W. I. Schmidt
- & Avni Malhotra
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Article
| Open AccessMercury deposition and redox transformation processes in peatland constrained by mercury stable isotopes
Mercury isotope signatures in groundwater, soil gas, solid peat, and atmosphere suggest that dark abiotic reduction of peat soil HgII to volatile Hg0 does not play a significant role in mobilizing Hg during peat mass loss
- Chuxian Li
- , Martin Jiskra
- & Kevin Bishop
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Article
| Open AccessA single site ruthenium catalyst for robust soot oxidation without platinum or palladium
Here, the authors report a study exploring surface lattice-confined single-atom ruthenium sites which demonstrate remarkable stability and exceptional catalytic performance for auto-exhaust purification, making them a promising alternative to costly Pt/Pd-based catalysts.
- Yuanfeng Li
- , Tian Qin
- & Jian Liu
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Article
| Open AccessCatalytic ozonation mechanism over M1-N3C1 active sites
Understanding the atomic-level structure-activity relationship in catalytic ozonation is crucial. Here, the authors reveal single-metal-atom-dependent catalytic ozonation and identify surface atomic oxygen reactivity as a descriptor in this relationship.
- Dingren Ma
- , Qiyu Lian
- & Jiaguo Yu
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Article
| Open AccessDissolved organic matter thiol concentrations determine methylmercury bioavailability across the terrestrial-marine aquatic continuum
Methylmercury is a strong neurotoxin that accumulates in aquatic biota. Here, the authors demonstrate that the concentration of thiol compounds associated with dissolved organic matter controls the bioavailability of methylmercury in aquatic systems
- Emily Seelen
- , Van Liem-Nguyen
- & Erik Björn
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Article
| Open AccessEnhanced and synergistic catalytic activation by photoexcitation driven S−scheme heterojunction hydrogel interface electric field
The regulation of heterogeneous material properties to enhance the peroxymonosulfate activation remains a challenge. Here, authors synthesize S−scheme heterojunction PBA/MoS2@chitosan hydrogel to achieve photoexcitation synergistic peroxymonosulfate activation driven by interface electric field.
- Aiwen Wang
- , Meng Du
- & Wei Wang
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Article
| Open AccessUnveiling the spatially confined oxidation processes in reactive electrochemical membranes
Understanding oxidation processes in reactive electrochemical membranes is essential for addressing environmental concerns. The authors highlight that microchannel pore size can profoundly impact not only the reaction kinetics but also the electron transfer pathways.
- Yuyang Kang
- , Zhenao Gu
- & Jiuhui Qu
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Article
| Open AccessMolecular imprinting-based indirect fluorescence detection strategy implemented on paper chip for non-fluorescent microcystin
Fluorescence analysis is a fast and sensitive method for the trace detection of environmental toxins, but it remains challenging to develop a fluorescence method for detecting nonfluorescent toxins. Here, the authors report an indirect fluorescent sensing strategy for the rapid, selective and sensitive detection of the non-fluorescent microcystin as a model target.
- Bowei Li
- , Ji Qi
- & Lingxin Chen
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Article
| Open AccessChar dominates black carbon aerosol emission and its historic reduction in China
Black carbon (BC) is distinguished into two parts (char vs soot) in emission sources and inventories, char is revealed as the core component of China’s historical emissions and the optimal target for future BC reductions.
- Junjie Cai
- , Hongxing Jiang
- & Gan Zhang
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Article
| Open AccessIntegrated urban water management by coupling iron salt production and application with biogas upgrading
Effective urban water management requires technological solutions that enable system-wide gains via a holistic approach. Here, authors propose an integrated system where an iron-oxidising electrochemical cell upgrades biogas while producing FeCO3 and subsequently uses the salt in wastewater treatment.
- Zhetai Hu
- , Lanqing Li
- & Zhiguo Yuan
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Article
| Open AccessHigh-temperature electrothermal remediation of multi-pollutants in soil
Soil contamination is a pressing environmental concern due to increasing anthropogenic activity. Here, the authors developed a rapid and energy-efficient electrothermal process that simultaneously removes heavy metals and organic pollutants in soil.
- Bing Deng
- , Robert A. Carter
- & James M. Tour
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Article
| Open AccessHydrolase mimic via second coordination sphere engineering in metal-organic frameworks for environmental remediation
Enzymatic degradation of pollutants under mild conditions is promising for efficient degradation of environmental contaminants under facile operation conditions, but natural enzymes tend to lose enzymatic activity in environmental application scenarios. Here, the authors report a metal-organic frameworks-based artificial enzyme system to achieve high hydrolytic activity under mild conditions.
- Xin Yuan
- , Xiaoling Wu
- & Wenyong Lou
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Matters Arising
| Open AccessUncertainty and bias in Liggio et al. (2019) on CO2 emissions from oil sands operations
- Long Fu
- & Allan H. Legge
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Comment
| Open AccessGuidelines for measuring and reporting particle removal efficiency in fibrous media
Adopting standardized and reliable methodologies to accurately measure particle removal efficiency when developing fibrous materials for controlling airborne contamination is crucial. Here, the authors recommend best practices for experimental assessments and reporting to ensure a reliable evaluation of new airborne particle filtration media and technologies.
- Paolo Tronville
- , Vincenzo Gentile
- & Jesus Marval
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Article
| Open AccessMimicking reductive dehalogenases for efficient electrocatalytic water dechlorination
Designing electrocatalysts for water treatment with high activity/selectivity as elaborately as natural enzymes remains a challenge. This work presents the design of electrocatalysts by mimicking the binding pocket configuration and active center of dehalogenases, achieving efficient water dechlorination.
- Yuan Min
- , Shu-Chuan Mei
- & Yujie Xiong
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Article
| Open AccessEfficient and selective capture of thorium ions by a covalent organic framework
Covalent organic frameworks are used in capture of radioactive ions but achieving high separation factors remains challenging. Here, the authors design an ionic COF its neutral non-ionic to better understand the role of different N sites on the selective capture of Th(IV) and report remarkable separation factors ranging from 102 to 105.
- Xiaojuan Liu
- , Feng Gao
- & Guoan Ye
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Article
| Open AccessEffects of drought and recovery on soil volatile organic compound fluxes in an experimental rainforest
Pugliese et al., show that severe drought and rewetting have a major impact on the capacity of rainforest soil to consume and emit volatile organic compounds (VOCs), affecting the atmospheric VOC budget and thereby atmospheric chemistry and climate.
- Giovanni Pugliese
- , Johannes Ingrisch
- & Jonathan Williams
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Article
| Open AccessRapid self-heating synthesis of Fe-based nanomaterial catalyst for advanced oxidation
There is an urgent need to develop efficient Fe-based catalysts for the organic pollutant degradation. Here, the authors develop an iron-based nanomaterial catalyst via flash joule heating. This catalyst exhibits strong energy efficient catalytic performance over a wide pH range and is potentially scalable.
- Fengbo Yu
- , Chao Jia
- & Xiangdong Zhu
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Article
| Open AccessMolecular rearrangement of bicyclic peroxy radicals is a key route to aerosol from aromatics
The oxidation of aromatics contributes significantly to the formation of atmospheric aerosol. Using toluene as an example the authors demonstrate a molecular rearrangement channel in the oxidation mechanism and show that the bicyclic peroxy radicals are much less stable than previously thought and can lead to aerosol-forming low-volatility products with up to 9 oxygen atoms on sub-second timescales
- Siddharth Iyer
- , Avinash Kumar
- & Matti Rissanen
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Article
| Open AccessDirect sulfuric acid formation from the gas-phase oxidation of reduced-sulfur compounds
Experiments verify that oxidation of organic sulphur compounds, such as DMS, directly yields gas-phase H2SO4. Simulations reveal that this pathway can be competitive with SO2 oxidation over oceans in the Southern Hemisphere.
- Torsten Berndt
- , Erik H. Hoffmann
- & Hartmut Herrmann
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Article
| Open AccessRiver export of macro- and microplastics to seas by sources worldwide
Modelling of riverine plastic exports finds microplastics dominate in areas with many sewage systems and macroplastics where waste is mismanaged. In some areas both plastics are important. Reduction at source is needed.
- Maryna Strokal
- , Paul Vriend
- & Tim van Emmerik
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Article
| Open AccessFacilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production
A graphene/mesoporous carbon composite presents rapid and efficient H2O2 electrosynthesis capability by two-electron oxygen reduction catalysis which is facilitated by the presence of multiple pyrrolic nitrogen dopants within the material.
- Wei Peng
- , Jiaxin Liu
- & Ji Liang
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Article
| Open AccessSynthesis of propenone-linked covalent organic frameworks via Claisen-Schmidt reaction for photocatalytic removal of uranium
The synthesis of sp2 carbon-conjugated covalent organic frameworks is limited to a few reactions and monomers due to the poor irreversibility of carbon double bonds. Here the authors synthesize propenone-linked covalent organic frameworks for the removal of radionuclide uranium from mine wastewater samples.
- Cheng-Peng Niu
- , Cheng-Rong Zhang
- & Jian-Ding Qiu
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Article
| Open AccessCovalent organic frameworks for direct photosynthesis of hydrogen peroxide from water, air and sunlight
Solar-driven photosynthesis is a green and sustainable process for hydrogen peroxide production. Here the authors report that optimizing the intramolecular polarity of COFs can greatly boost H2O2 photosynthesis from water, air, and sunlight.
- Fuyang Liu
- , Peng Zhou
- & Jinren Ni
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Article
| Open AccessOptimal reactive nitrogen control pathways identified for cost-effective PM2.5 mitigation in Europe
Reactive nitrogen (Nr) contributes strongly to PM2.5 air pollution in Europe. Here, authors identify diverse Nr control pathways for Europe depending on emission and pollution formation and a priority of NH3 control when costs are considered.
- Zehui Liu
- , Harald E. Rieder
- & Lin Zhang
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Article
| Open AccessMass spectrometry imaging for biosolids characterization to assess ecological or health risks before reuse
Mass spectrometry imaging is a suitable tool for the analysis of non-cohesive materials. Here, authors show that it can be used to detect persistent organic pollutants (POPs) and heavy metals (HMs) in biosolids using small amounts of material with speed and safety.
- Claire Villette
- , Loïc Maurer
- & Dimitri Heintz
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Article
| Open AccessDiscovery and mechanism-guided engineering of BHET hydrolases for improved PET recycling and upcycling
The degradation of PET using PETase enzymes has great potential but can face problems with incomplete degradation. Here, the authors identified two BHETases from the environment and engineered them to improve their hydrolysis efficiency for applications in dual-enzyme PET recycling and tandem chemical-enzymatic PET upcycling systems.
- Anni Li
- , Yijie Sheng
- & He Huang
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Article
| Open AccessDual-bionic superwetting gears with liquid directional steering for oil-water separation
Developing efficient separation methods for oily wastewater holds significant global importance. In this study, the authors combine supewettability and bio-inspired topological structures to demonstrate a dual-bionic superwetting gear system with liquid directional steering to achieve oil-water separation.
- Zhuoxing Liu
- , Zidong Zhan
- & Zhichao Dong
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Article
| Open AccessOccurrence and backtracking of microplastic mass loads including tire wear particles in northern Atlantic air
Microplastics the marine atmosphere are a highly relevant subject, yet barely investigated. This study showed their ubiquity in the nanogram range even in remote Artic regions and depict the ocean acts as both a sink and source for microplastics
- Isabel Goßmann
- , Dorte Herzke
- & Barbara M. Scholz-Böttcher
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Article
| Open AccessIndustrial source identification of polyhalogenated carbazoles and preliminary assessment of their global emissions
Recognition on sources of polyhalogenated carbazoles is needed to understand their environmental accumulation. Here, release of polyhalogenated carbazoles from 13 industries including 122 plants is identified and estimated.
- Yuxiang Sun
- , Lili Yang
- & Guorui Liu
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Article
| Open AccessDynamic active-site induced by host-guest interactions boost the Fenton-like reaction for organic wastewater treatment
Uncovering the dynamic evolution of active sites in the working conditions is crucial to realizing increased activity and enhanced stability of catalyst in Fenton-like activation. Herein, the authors capture the dynamic changes in the unit cell of Co/La-SrTiO3 catalyst during the exemplary peroxymonosulfate activation process.
- Dongpeng Zhang
- , Yanxiao Li
- & Sihui Zhan
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Article
| Open AccessReverse oxygen spillover triggered by CO adsorption on Sn-doped Pt/TiO2 for low-temperature CO oxidation
Reverse O spillover has opened new opportunities in improving the catalytic activity and selectivity in various reactions. Herein Sn is doped into TiO2 to activate low-temperature (<100 °C) reverse oxygen spillover in Pt/TiO2 catalyst, leading to enhanced CO oxidation activity.
- Jianjun Chen
- , Shangchao Xiong
- & Junhua Li
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Article
| Open AccessNO at low concentration can enhance the formation of highly oxygenated biogenic molecules in the atmosphere
Nitrogen monoxide at low concentrations can promote the formation of highly oxygenated organic molecules, which are crucial precursors to secondary organic aerosol (SOA), rather than inhibit it as traditionally thought.
- Wei Nie
- , Chao Yan
- & Aijun Ding
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Article
| Open AccessWater decontamination via nonradical process by nanoconfined Fenton-like catalysts
There is an urgent need to develop effective heterogeneous Fenton-like catalysts for water treatment. Here, the authors demonstrate that nanoconfinement of cobalt oxide catalysts in carbon nanotubes can selectively degrade pollutants at high reaction rate.
- Tongcai Liu
- , Shaoze Xiao
- & Yalei Zhang
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Article
| Open AccessComparing ecosystem gaseous elemental mercury fluxes over a deciduous and coniferous forest
Forests are sinks for the neurotoxic mercury, but the sinks have large uncertainties. Our direct gaseous elemental mercury (GEM) exchange measurements show that GEM exchange includes complex patterns of multiple pathways to different ecosystem compartments varying over time
- Jun Zhou
- , Silas W. Bollen
- & Daniel Obrist
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Article
| Open AccessSurface manipulation for prevention of migratory viscous crude oil fouling in superhydrophilic membranes
Minimizing membrane fouling is critical for their continuous and efficient operation. Here, authors demonstrate a wrinkled-pattern microparticles-decorated membrane surface can increase contact area with water molecules, expand steric hindrance, and inhibit adhesion and deposition of oil, achieving efficient migratory viscous crude oil antifouling.
- Yuanyuan Zhao
- , Xiaobin Yang
- & Lu Shao
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Article
| Open AccessInterplay between copper redox and transfer and support acidity and topology in low temperature NH3-SCR
Support Brønsted acid strength and density play important kinetically relevant roles in low temperature NH3-SCR over Cu-exchanged small pore zeolite catalysts. Here the authors demonstrate Brønsted acid sites facilitate hydrolysis and intercage transfer of CuII(NH3)4 intermediates.
- Yiqing Wu
- , Wenru Zhao
- & Feng Gao
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Article
| Open AccessTriboelectric-induced ion mobility for artificial intelligence-enhanced mid-infrared gas spectroscopy
Isopropyl alcohol can play a significant role in anti-virus diagnosis but generally yields limited response in conventional detection. Here, authors propose a methodology of AI-enhanced ion mobility and mid-infrared spectroscopy for accurate gas identification despite presence different carbon-based gases.
- Jianxiong Zhu
- , Shanling Ji
- & Chengkuo Lee
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Article
| Open AccessCentennial scale sequences of environmental deterioration preceded the end-Permian mass extinction
The exact drivers for the end-Permian mass extinction remain controversial. This study reveals a turning point with the exhaustion of the terrestrial input and a strong fertilization of the marine realm leading to the demise of marine ecosystems.
- Ryosuke Saito
- , Lars Wörmer
- & Kai-Uwe Hinrichs
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Article
| Open AccessHigh-density frustrated Lewis pairs based on Lamellar Nb2O5 for photocatalytic non-oxidative methane coupling
To achieve efficient photocatalytic non-oxidative methane coupling, a strong polarization environment with abundant activation sites for C-H scissoring is needed. This can be created through the fabrication of high-density frustrated Lewis pairs on lamellar Nb2O5 using a thermal-reduction promoted phase-transition process.
- Ziyu Chen
- , Yutao Ye
- & Jinlong Zhang
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Article
| Open AccessOrganic matter degradation causes enrichment of organic pollutants in hadal sediments
Persistent organic pollutants (POPs) are found in hadal trench sediment in the Atacama trench at depths down to 8085 m. High turnover of organic matter in the trench contributes to elevated contaminant concentrations in this extreme and remote place.
- Anna Sobek
- , Sebastian Abel
- & Ronnie N. Glud
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Article
| Open AccessO2 partitioning of sulfur oxidizing bacteria drives acidity and thiosulfate distributions in mining waters
Microbial genomics is a widely under-utilized tool in mining in understanding water quality drivers. Here the authors show early acid generation and thiosulfate concentrations are driven by O2 dependent microbial sulfur oxidizing bacterial niches in a mine tailings impoundment
- Kelly J. Whaley-Martin
- , Lin-Xing Chen
- & Lesley A. Warren
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Article
| Open AccessPredictability of fossil fuel CO2 from air quality emissions
The historical changes in country emissions of greenhouse gases and air quality pollutants are classified together as a function of economic development, providing valuable guidance to emission scenario development.
- Kazuyuki Miyazaki
- & Kevin Bowman
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Article
| Open AccessIn situ acid etching boosts mercury accommodation capacities of transition metal sulfides
There is an urgent need to develop efficient strategies to remove elemental mercury from industrial flue gases. Here the authors develop a simple, versatile, and scalable strategy to obtain a 100-fold enhancement of the elemental mercury accommodation capacities of a wide range of transition metal sulfides by in situ acid etching.
- Hailong Li
- , Jiaoqin Zheng
- & Zequn Yang
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Article
| Open AccessMixed-valence molybdenum oxide as a recyclable sorbent for silver removal and recovery from wastewater
Silver ions in wastewater are a major health hazard, and there is an urgent need to develop methods to reliably extract them. Here, the authors show that mixed-valence molybdenum oxide can selectively adsorb and reduce Ag+ from wastewater and be easily recycled while maintaining high selectivity towards Ag+.
- Penghui Shao
- , Ziwen Chang
- & Liming Yang