PMID- 33179941
OWN - NLM
STAT- PubMed-not-MEDLINE
DCOM- 20201207
LR  - 20201214
IS  - 1948-7185 (Electronic)
IS  - 1948-7185 (Linking)
VI  - 11
IP  - 23
DP  - 2020 Dec 3
TI  - Single-Molecule Sensing of Interfacial Acid-Base Chemistry.
PG  - 10023-10028
LID - 10.1021/acs.jpclett.0c03010 [doi]
AB  - Bronsted acid and base interactions are a cornerstone of chemistry describing a 
      wide range of chemical phenomena. However, probing such interaction at the 
      solid-liquid interface to extract the elementary and intrinsic information at a 
      single-molecule level remains a big challenge. Herein, we employ an STM break 
      junction (STM-BJ) technique to investigate the acid-base chemistry of carboxylic 
      acid-based molecules at a Au (111) model surface and propose a prototype of a 
      single-molecule pH sensor for the first time. The single-molecule measurements in 
      different environmental conditions verify that the formation probability of 
      molecular junctions is determined by the populations of deprotonated -COO(-) form 
      in a self-assembled monolayer. Furthermore, the variation of the intensity of the 
      conductance peaks (i.e., junction-forming probability) with the pH of the bulk 
      solution fits well to the Henderson-Hasselbalch type equation. From the equation, 
      a good linear relation is found between the degree of dissociation of the 
      immobilized -COOH group and the environmental pH, providing a feasible way to 
      design chemicals and biosensors and a detector at the single-molecule scale.
FAU - Tao, Cai-Ping
AU  - Tao CP
AD  - Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, 
      Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, 
      China.
FAU - Jiang, Chen-Chen
AU  - Jiang CC
AD  - Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, 
      Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, 
      China.
FAU - Wang, Ya-Hao
AU  - Wang YH
AUID- ORCID: 0000-0001-5943-8646
AD  - Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, 
      Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, 
      China.
FAU - Zheng, Ju-Fang
AU  - Zheng JF
AD  - Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, 
      Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, 
      China.
FAU - Shao, Yong
AU  - Shao Y
AUID- ORCID: 0000-0003-0834-6244
AD  - Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, 
      Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, 
      China.
FAU - Zhou, Xiao-Shun
AU  - Zhou XS
AUID- ORCID: 0000-0003-1673-8125
AD  - Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, 
      Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, 
      China.
LA  - eng
PT  - Journal Article
DEP - 20201112
PL  - United States
TA  - J Phys Chem Lett
JT  - The journal of physical chemistry letters
JID - 101526034
SB  - IM
EDAT- 2020/11/13 06:00
MHDA- 2020/11/13 06:01
CRDT- 2020/11/12 12:09
PHST- 2020/11/13 06:00 [pubmed]
PHST- 2020/11/13 06:01 [medline]
PHST- 2020/11/12 12:09 [entrez]
AID - 10.1021/acs.jpclett.0c03010 [doi]
PST - ppublish
SO  - J Phys Chem Lett. 2020 Dec 3;11(23):10023-10028. doi: 
      10.1021/acs.jpclett.0c03010. Epub 2020 Nov 12.