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Record W4388775310 · doi:10.1021/acscatal.3c03884

Manipulating the Optically Active Defect–Defect Interaction of Colloidal Quantum Dots for Carbon Dioxide Photoreduction

2023· article· en· W4388775310 on OpenAlexaff
Mengke Cai, Xin Tong, Peisen Liao, Shujie Shen, Hongyang Zhao, Xin Li, Xia Li, Huaqian Zhi, Nan Zhou, Ziqian Xue, Lei Jin, Jieyuan Li, Guangqin Li, Fan Dong, Andrei V. Kabashin, Zhiming M. Wang

Bibliographic record

VenueACS Catalysis · 2023
Typearticle
Languageen
FieldMaterials Science
TopicQuantum Dots Synthesis And Properties
Canadian institutionsInstitut National de la Recherche Scientifique
FundersNational Key Research and Development Program of ChinaYoung Scientists FundSichuan Province Science and Technology Support ProgramHigher Education Discipline Innovation ProjectNatural Science Foundation for Young Scientists of Shanxi ProvinceEast China Normal UniversityNational Natural Science Foundation of China
KeywordsQuantum dotCopperMaterials scienceVacancy defectPhotocatalysisPhotochemistryCharge carrierChemical physicsExcitonDensity functional theoryAbsorption (acoustics)PhotoluminescenceOptoelectronicsNanoparticleDopingCatalysisNanotechnologyMolecular physicsChemistryComputational chemistryCrystallographyCondensed matter physicsPhysics

Abstract

fetched live from OpenAlex

Defect engineering in colloidal quantum dots (QDs), a typical photocatalytic material, is promising to tailor optoelectronic properties and achieve solar-to-fuel energy conversion. However, understanding the effect of defect–defect interactions on both charge carrier and catalytic dynamics is still challenging. Here, we report a class of defect-engineered copper-deficient Zn-doped CuInS 2 (ZCIS) QDs that synergistically utilize copper vacancy and Cu 2+ defect states to realize CO 2 photoreduction. Steady and transient optical characterizations reveal that the density of copper vacancy can manipulate the distribution of optically active Cu + and Cu 2+ defect states (appearing as Cu In ″ and Cu Cu • species, respectively), wherein the Cu + defect states suppress interband absorption and sharpen the Shockley–Read–Hall recombination, while Cu 2+ defect states enable the prolonged exciton lifetime of QDs. In situ infrared spectroscopic investigation and theoretical density functional calculation demonstrate the photoactive Cu 2+ defect states nearby the copper vacancy in ZCIS QDs can effectively activate CO 2 to the COOH* intermediates, leading to a remarkable photocatalytic CO production rate up to 532.3 μmol g –1 h –1 (turnover number ∼1963) after 120 h illumination.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

Full frame distilled prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.

metaresearch head score (Codex)0.001
metaresearch head score (Gemma)0.001
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.006
Threshold uncertainty score0.416

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0000.000

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.037
GPT teacher head0.277
Teacher spread0.240 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Classification

machine, unvalidated

Machine predicted; a candidate call from one teacher head, not a consensus.

The models applied no category: nothing in the taxonomy fit this work.
Study designBench or experimental
Domainnot available
GenreEmpirical

How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".

Quick stats

Citations28
Published2023
Admission routes1
Has abstractyes

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